NOVEL PYROLINONE DERIVATIVE AND PHARMACEUTICAL COMPOSITION COMPRISING THE SAME

TECHNICAL FIELD

The invention relates to P2X receptor, specifically to a compound useful for the treatment of diseases or conditions associated with a P2X₃receptor, specifically to a P2X₃and/or P2X₂/₃receptor, and a pharmaceutical composition comprising such compound.

BACKGROUND ART

ATP (adenosine triphosphate) is known to serve as a source of energy in cells and a substrate of phosphorylation, as well as an extracellular messenger. It is known that ATP is released from a cell by various stimulation such as cellular injury, inflammation, nociceptive stimulus, reduced blood oxygen level, and also known to be released together with another messenger from a primary sensory nerve terminal. ATP thus released mediates various extracellular signal transductions through an ATP receptor (Non-Patent Document 6, Non-Patent Document 7).

ATP receptor is categorized into ionotropic P2X family and G protein-coupled P2Y family. For P2X family, seven subtypes have been reported, and a member of this family forms a homo-trimeric structure or a hetero-trimeric structure together with another member of this subtype and functions as a non-specific cation channel (Non-Patent Document 8).

ATP is known to cause pain, and studies with P2X₃knockout and knockdown methodologies have shown that P2X₃receptor mediates transmission of chronic pain. P2X₃receptors are expressed in a specific manner on peripheral sensory nerve to form a homo-complex or hetero-complex with P2X₂(P2X₂/₃) (Non-Patent Document 1).

Later, the compound A-317491 was reported as a specific antagonist to P2X₃and P2X₂/₃receptors. A-317491 is tri-substituted-N-[(1S)-1,2,3,4-tetrahydro-1-naphthalenyl]benzamide derivative represented by the formula:

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(Patent Document 1). It was reported to exhibit an antagonist activity to P2X₃and P2X₂/₃receptors and analgesic action in neuropathic pain model and inflammatory pain model (Non-Patent Document 9). This indicates that pain sensation is transmitted via P2X₃or P2X₂/₃receptor and that a P2X₃or P2X₂/₃receptor antagonist is useful as an analgesic. Also, compounds that exhibit P2X₃or P2X₂/₃receptor antagonizing effect are described in Patent Documents 2-7.

Additionally, it was recently reported that vesical reflex was strongly reduced in P2X₃knockout mouse (Non-Patent Document 2), suggesting that a P2X₃antagonist is useful in the treatment of diseases caused by overactive bladder.

Patent document 12 discloses that the compounds having similar chemical structures to the compound of the invention, however, does not disclose that the compounds having an analgesic effect and a P2X₃or P2X₂/₃receptor antagonizing effect. Non-Patent documents 3, 4, 10, and 11 disclose that the compounds having similar chemical structures to the compound of the invention and an analgesic effect, however, does not disclose that the compound having a P2X₃or P2X₂/₃receptor antagonizing effect.

[Patent Document 1] WO02/094767
[Patent Document 2] WO2005/095359
[Patent Document 3] US20070037974
[Patent Document 4] US20070049758
[Patent Document 5] US20070049610
[Patent Document 6] US20070049609
[Patent Document 7] US20070049534
[Non-Patent Document 1] Neuroscientist 11 (2005) pp. 345-356
[Non-Patent Document 2] J. Physiol. 567.2 (2005) pp. 621-639
[Non-Patent Document 3] Pharmaceutical Chemistry Journal Vol. 39, No. 9, (2005), pp 484-487
[Non-Patent Document 4] Pharmaceutical Chemistry Journal Vol. 31, No. 5, (1997), pp 251-254
[Non-Patent Document 5] Expert Opin. Ther. Patens (2006) 16(8) 113-1127.
[Non-Patent Document 6] J. Physiology (2003), 554(2), 301-308
[Non-Patent Document 7] J. Physiology (2003), 553(3), 683-694
[Non-Patent Document 8] Pflungers Arch Eur J physiol (2006), 452, 513-537
[Non-Patent Document 9] PNAS (2002), 99(26), 17179-17184
[Non-Patent Document 10] Khimiko-Farmatsevticheskii Zhurnal, Vol 31, No. 11, (1997) 35-36
[Non-Patent Document 11] Pharmaceutical Chemistry Journal Vol 36, No. 4, (2002), 188-191
[Non-Patent Document 12] Phosphorus, Sulfur and Silicon and the Related Elements (2006), 181(4), 771-777

DISCLOSURE OF INVENTION
Problems to be Resolved by the Invention

The present invention provides a novel P2X₃and/or P2X₂/₃receptor antagonist.

Means of Solving the Problems

During studies to solve the problems described above, the inventors have discovered novel compounds that bind specifically to P2X₃and/or P2X₂/₃receptor and exhibit an antagonizing effect, and thus, achieved the inventions described bellow.

(1) A compound represented by the formula (I):

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wherein

Z¹is optionally protected hydroxy or optionally protected mercapto;

Z²is —C(═O)—, —C(═S)— or —S(O)v-, or

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wherein R^5aand R^5bare each independently hydrogen or lower alkyl;

R⁶is hydrogen, substituted or unsubstituted lower alkyl, substituted or unsubstituted acyl or substituted or unsubstituted lower alkoxycarbonyl;

p is an integer of 0 to 2;

v is an integer of 0 to 2;

Z^3aand Z^3bare each independently hydrogen, substituted or unsubstituted lower alkyl, or taken together ═O or ═S;

t is an integer of 0 to 4;

R^4aand R^4bare each independently, hydrogen or substituted or unsubstituted lower alkyl;

m and n are each independently an integer of 0 to 2;

k is an integer of 0 or 1;

Ring A is cycloalkane, cycloalkene, an aromatic carbocyclic ring or a heterocyclic ring;

B is cycloalkene-diyl, cycloalkene-diyl, aromatic carbocyclic ring-diyl or heterocyclic ring-diyl;

R^1aand R^1bare each independently halogen, hydroxy, substituted or unsubstituted lower alkyl, substituted or unsubstituted lower alkenyl, substituted or unsubstituted lower alkynyl, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkylthio, substituted or unsubstituted acyl, carboxy, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted carbamoyl, substituted or unsubstituted thiocarbamoyl, substituted or unsubstituted amino, substituted sulfinyl, substituted sulfonyl, substituted or unsubstituted sulfamoyl, cyano, nitro or —C(R^7a)═N—O—R^7b;

R^7aand R^7bare each independently hydrogen or substituted or unsubstituted lower alkyl;

R²is substituted or unsubstituted alkyl, substituted or unsubstituted alkenyl, substituted or unsubstituted alkynyl, substituted or unsubstituted alkoxy, substituted or unsubstituted aryloxy, hydroxy, substituted or unsubstituted amino, substituted or unsubstituted cycloalkyl, substituted or unsubstituted cycloalkenyl, substituted or unsubstituted aryl or a substituted or unsubstituted heterocyclic group;

R³is substituted or unsubstituted alkyl, substituted or unsubstituted alkoxycarbonyl, substituted or unsubstituted aryloxycarbonyl, carboxy, substituted or unsubstituted carbamoyl, substituted or unsubstituted cycloalkyl, substituted or unsubstituted cycloalkenyl, substituted or unsubstituted aryl or a substituted or unsubstituted heterocyclic group;

provided that a compound of the following (i) to (viii) is excluded;

(i) a compound wherein Ring A is thiadiazole, k is 0 and R^1ais methylthio;

(ii) a compound wherein Ring A is benzothiophene, k is 0, R^1ais methylsulfonyl and R²is substituted or unsubstituted furyl or substituted or unsubstituted phenyl;

(iii) a compound wherein Ring A is thiazole or 7H-purine, and R²is substituted or unsubstituted furyl;

(iv) a compound wherein R³is a group represented by the formula:

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t is an integer of 1 to 2 and Ring A is furan or benzene;

(v) a compound wherein R²is t-butyl or 4-methyloxyphenyl;

(vi) a compound wherein R²is substituted or unsubstituted alkyl provided that substituted or unsubstituted i-propyl and substituted or unsubstituted i-butyl are excluded, R³is a substituted or unsubstituted carbocyclic ring or a substituted or unsubstituted heterocyclic ring, and k is 0;

(vii) a compound wherein R²is substituted or unsubstituted cycloalkyl, substituted or unsubstituted cycloalkenyl, substituted or unsubstituted aryl or a substituted or unsubstituted heterocyclic group, and R³is pentane-3-yl; and

(viii) a compound represented by the formula:

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or its pharmaceutically acceptable salt, or a solvate thereof.

(2) The compound according to the above (1), wherein R²is a group represented by the formula:

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wherein Me is methyl, q is an integer of 0 to 4; and

R³is a group represented by the formula:

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wherein Y is hydroxy, halogen, cyano, carboxy, substituted or unsubstituted lower alkyl, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted acyl, substituted or unsubstituted carbamoyl, substituted or unsubstituted thiocarbamoyl, substituted or unsubstituted lower alkylthio, substituted or unsubstituted lower alkylsulfamoyl, substituted or unsubstituted amino, substituted sulfinyl, substituted sulfonyl or a substituted or unsubstituted heterocyclic group, or Y and R¹⁴may form a substituted or unsubstituted heterocyclic group with adjacent carbon atom;

R¹⁴is halogen, hydroxy, substituted or unsubstituted lower alkyl, substituted or unsubstituted lower alkenyl, substituted or unsubstituted lower alkynyl, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkylthio, substituted or unsubstituted acyl, carboxy, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted carbamoyl, substituted or unsubstituted amino, substituted or unsubstituted sulfamoyl, cyano or nitro; and

r is an integer of 0 to 2, or its pharmaceutically acceptable salt, or a solvate thereof.

(2′) A compound represented by the formula (I);

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wherein

Z¹is optionally protected hydroxy or optionally protected mercapto;

Z²is —C(═O)—, —C(═S)— or —S(O)v-, or

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wherein Me is methyl, q is an integer of 0 to 4;

R³is a group represented by the formula:

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wherein Y is hydroxy, halogen, cyano, carboxy, substituted or unsubstituted lower alkyl, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted acyl, substituted or unsubstituted carbamoyl, substituted or unsubstituted thiocarbamoyl, substituted or unsubstituted lower alkylthio, substituted or unsubstituted lower alkylsulfamoyl, substituted or unsubstituted amino, substituted sulfinyl, substituted sulfonyl or a substituted or unsubstituted heterocyclic group, or Y and R¹⁴may form a substituted or unsubstituted heterocyclic group with adjacent carbon atom;

R¹⁴is halogen, hydroxy, substituted or unsubstituted lower alkyl, substituted or unsubstituted lower alkenyl, substituted or unsubstituted lower alkynyl, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkylthio, substituted or unsubstituted acyl, carboxy, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted carbamoyl, substituted or unsubstituted amino, substituted or unsubstituted sulfamoyl, cyano or nitro; and

r is an integer of 0 to 2;

provided that the following compounds are excluded:

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or its pharmaceutically acceptable salt, or a solvate thereof.

(3) The compound according to the above (2) or (2′), wherein Z^3aand Z^3bare taken together ═O, or its pharmaceutically acceptable salt, or a solvate thereof.

(4) The compound according to any one of the above (2), (2′) or (3), wherein t is 0, or its pharmaceutically acceptable salt, or a solvate thereof.

(5) The compound according to any one of the above (2) to (4) or (2′), wherein Z²is —C(═O)—, —C(═S)— or —S(O)₂—, or its pharmaceutically acceptable salt, or a solvate thereof.

(6) The compound according to any one of the above (2) to (5) or (2′), wherein Z²is —C(═O)—, or its pharmaceutically acceptable salt, or a solvate thereof.

(7) The compound according to any one of the above (2) to (6) or (2′), wherein the group represented by the formula:

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wherein Z¹, Z²and R²are as defined in the above (1), is a group represented by the formula:

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wherein. R², R^5a, R^5b, R⁶, and p are as defined in the above (1), or its pharmaceutically acceptable salt, or a solvate thereof.

(8) The compound according to any one of the above (2) to (6) or (2′), wherein the group represented by the formula:

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wherein Z¹, Z², Z^3a, Z^3b, R², and R³are as defined in the above (1), is a group represented by the formula:

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wherein Z¹, Z², Z^3a, Z^3b, R²and R³are as defined in the above (1), or its pharmaceutically acceptable salt, or a solvate thereof.

(9) A compound represented by the formula (I):

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wherein Z¹, Z², Z^3a, Z^3b, R^1a, R^1b, R², R³, R^4a, R^4b, Ring A, B, h, m, n, and t are as defined in the above (1), or its pharmaceutically acceptable salt, or a solvate thereof; is

a compound represented by the formula (I′);

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wherein

Z¹′ is optionally protected hydroxy or optionally protected mercapto;

Z²′ is O or S, or

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wherein R^5a′ and R^5b′ are each independently hydrogen or lower alkyl;

R⁶is hydrogen, substituted or unsubstituted lower alkyl, substituted or unsubstituted acyl or substituted or unsubstituted lower alkoxycarbonyl;

p′ is an integer of 0 to 2;

t′ is an integer of 0 to 4;

R^4a′ and R^4b′ are each independently hydrogen or lower alkyl;

m′ and n′ are each independently an integer of 0 to 2;

Ring A′ is cycloalkane, cycloalkene, an aromatic carbocyclic ring or a heterocyclic ring;

B′ is cycloalkane-diyl, cycloalkene-diyl, aromatic carbocyclic ring-diyl or heterocyclic ring-diyl;

when n′ is 0, B′ may be methylthio, trifluoromethylthio, or —C(R^7a′)═N—O—R^7b′;

R^1a′ and R^1b′ are each independently halogen, hydroxy, substituted or unsubstituted lower alkyl, substituted or unsubstituted lower alkenyl, substituted or unsubstituted lower alkynyl, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkylthio, substituted or unsubstituted acyl, carboxy, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted carbamoyl, substituted or unsubstituted amino, substituted or unsubstituted sulfamoyl, cyano, or nitro;

R²′ and R³′ are each independently substituted or unsubstituted alkyl, substituted or unsubstituted cycloalkyl, substituted or unsubstituted cycloalkenyl, substituted or unsubstituted aryl or a substituted or unsubstituted heterocyclic group;

R^7a′ and R^7b′ are each independently hydrogen or substituted or unsubstituted lower alkyl;

provided that a compound wherein Ring A′ is thiadiazole and B′ is methylthio is excluded,

or its pharmaceutically acceptable salt, or a solvate thereof.

(10) The compound according to the above (9), wherein R³′ is a group represented by the formula:

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wherein Ring C′ is a substituted or unsubstituted aromatic carbocyclic ring or a substituted or unsubstituted aromatic heterocyclic ring;

Y′ is —O—, —S—, or —NR⁹′—;

R⁹′ is hydrogen or lower alkyl;

Z′ is hydroxy, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkylthio, substituted or unsubstituted acyl, carboxy, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted carbamoyl, substituted or unsubstituted amino, substituted or unsubstituted lower alkylsulfinyl, substituted or unsubstituted alkylsulfamoyl or cyano;

R^8a′ and R^8b′ are each independently hydrogen or substituted or unsubstituted lower alkyl;

s′ is an integer of 1 to 4,

or its pharmaceutically acceptable salt, or a solvate thereof.

(11) The compound according to the above (9) or (10), wherein Y′ is —O—, or its pharmaceutically acceptable salt, or a solvate thereof.

(12) The compound according to any one of the above (9) to (11), wherein t′ is 0, or its pharmaceutically acceptable salt, or a solvate thereof.

(13) The compound according to any one of the above (9) to (12), wherein a group represented by the formula:

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t′ and p′ are 0;

R²is a group represented by the formula:

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wherein R^10a′ and R^10b′ are each independently hydroxy, halogen, substituted or unsubstituted alkyl, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkoxycarbonyl, carboxy, substituted or unsubstituted carbamoyl, substituted or unsubstituted cycloalkyl, substituted or unsubstituted cycloalkenyl, substituted or unsubstituted aryl, a substituted or unsubstituted heterocyclic group, or R^10a′ and R^10b′ are taken together may form a substituted or unsubstituted non-aromatic carbocyclic ring or a substituted or unsubstituted non-aromatic heterocyclic ring with an adjacent carbon atom;

R^10c′ is hydrogen, hydroxy, halogen, substituted or unsubstituted alkyl, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkoxycarbonyl, carboxy, substituted or unsubstituted lower alkylcarbamoyl, substituted or unsubstituted cycloalkyl, substituted or unsubstituted cycloalkenyl, substituted or unsubstituted aryl or a substituted or unsubstituted heterocyclic group;

R^11a′ and R^11b′ are each independently hydrogen or lower alkyl, or taken together ═O;

r′ is an integer of 0 to 4;

provided that a compound wherein all of R^10a′, R^10b′ and R^10c′ are methyl; and the following compounds;

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are excluded, or its pharmaceutically acceptable salt, or a solvate thereof.

(14) The compound according to the above (13), wherein R^10a′ and R^10b′ are lower alkyl, and R^10c′ is carboxy, hydroxyalkyl, substituted or unsubstituted aryl, substituted or unsubstituted heteroaryl, or substituted or unsubstituted lower alkylcarbamoyl, or its pharmaceutically acceptable salt, or a solvate thereof.

(15) The compound according to any one of the above (10) to (12), wherein is optionally protected hydroxy;

Z²′ is O;

R²′ is a group represented by the formula:

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wherein R^10a′ and R^10b′ are each independently hydroxy, halogen, substituted or unsubstituted alkyl, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkoxycarbonyl, carboxy, substituted or unsubstituted lower alkylcarbamoyl, substituted or unsubstituted cycloalkyl, substituted or unsubstituted cycloalkenyl, substituted or unsubstituted aryl, a substituted or unsubstituted heterocyclic group, or R^10a′ and R^10b′ are taken together may form a substituted or unsubstituted non-aromatic carbocyclic ring or a substituted or unsubstituted non-aromatic heterocyclic ring with an adjacent carbon atom;

R^10c′ is hydrogen, hydroxy, halogen, substituted or unsubstituted alkyl, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkoxycarbonyl, carboxy, substituted or unsubstituted lower alkylcarbamoyl, substituted or unsubstituted cycloalkyl, substituted or unsubstituted cycloalkenyl, substituted or unsubstituted aryl or a substituted or unsubstituted heterocyclic group;

R^11a′ and R^11b′ are each independently hydrogen or lower alkyl;

r′ is an integer of 0 to 4, or its pharmaceutically acceptable salt, or a solvate thereof.

(16) The compound according to any one of the above (10) to (12), wherein

Z¹′ is optionally protected hydroxy;

Z²′ is O;

R²′ is a group represented by the formula:

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wherein Ring D′ is a substituted or unsubstituted aromatic carbocyclic ring or a substituted or unsubstituted aromatic heterocyclic ring;

V′ is —C(═O)—, —O—C(═O)—, —NR¹³′—C(═O)—NR¹³′—, —NR¹³′—C(═O)—, —C(═O)—NR¹³′—, —O—, —S— or —NR¹³′—;

R¹³′ is hydrogen or lower alkyl;

W′ is hydroxy, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkylthio, substituted or unsubstituted acyl, carboxy, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted carbamoyl, substituted or unsubstituted amino, substituted or unsubstituted lower alkylsulfinyl, substituted or unsubstituted sulfamoyl, or cyano;

R^12a′ and R^12b′ are each independently hydrogen or substituted or unsubstituted lower alkyl;

u′ is an integer of 1 to 4;

provided that the following compounds:

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are excluded, or its pharmaceutically acceptable salt, or a solvate thereof.

(17) The compound according to the above (15) or (16), wherein t′ is 0, or its pharmaceutically acceptable salt, or a solvate thereof.

(18) A pharmaceutical composition comprising the compound according to any one of the above (1) to (17) or (2′), or its pharmaceutically acceptable salt, or a solvate thereof.

(19) A pharmaceutical composition having an antagonistic activity for P2X₃and/or P2X_2/3receptor, comprising the compound according to any one of the above (1) to (17) or (2′), or its pharmaceutically acceptable salt, or a solvate thereof.

(20) A method for preventing or treating a disease related to P2X₃and/or P2X_2/3receptor characterized by administration of the compound according to any one of the above (1) to (17) or (2′), or its pharmaceutically acceptable salt, or a solvate thereof.

(21) Use of the compound according to any one of the above (1) to (17) or (2′), or its pharmaceutically acceptable salt, or a solvate thereof for treating and/or preventing a disease related to P2X₃and/or P2X_2/3receptor.

(22) Use of the compound according to any one of the above (1) to (17) or (2′), or its pharmaceutically acceptable salt, or a solvate thereof in the manufacturing of an agent for treating and/or preventing a disease related to P2X₃and/or P2X_2/3receptor.

BEST MODE FOR CARRYING OUT THE INVENTION

As used throughout the specification, the following terms have the following meaning unless specifically indicated.

The term “alkyl” includes a straight or branched chain monovalent hydrocarbon group containing from 1 to 10, preferably from 1 to 8, more preferably from 1 to 6 carbons, such as methyl, ethyl, n-propyl, isopropyl, n-butyl, isobutyl, sec-butyl, tert-butyl, n-pentyl, isopentyl, neo-pentyl, n-hexyl, isohexyl, n-heptyl, isoheptyl, n-octyl, isooctyl, n-nonyl and n-decyl, and the like.

Preferable “alkyl” for R²is isopropyl, isobutyl, and the like.

The term “lower alkyl” includes a straight or branched chain monovalent hydrocarbon group containing from 1 to 6, preferably from 1 to 3 carbons, such as, methyl, ethyl, n-propyl, isopropyl, n-butyl, isobutyl, sec-butyl, tert-butyl, n-pentyl, isopentyl, neo-pentyl, n-hexyl, isohexyl, and the like.

Preferable “lower alkyl” for R^1ais C1-C4 alkyl such as methyl, ethyl, n-propyl, isopropyl, terl-butyl, and the like.

Preferable “lower alkyl” for R^1bis C1-C3 alkyl such as methyl, ethyl, and the like.

Preferable “lower alkyl” for Y is C1-C3 alkyl such as methyl, ethyl, n-propyl, isopropyl, and the like.

The term “acyl” includes a group of the formula R—CO—, wherein R is, for example, “lower alkyl” as defined above or “lower alkenyl”, “aryl”, “a heterocyclic group”, “cycloalkyl” or “cycloalkenyl” as defined bellow.

Preferable “acyl” for R^1ais C1-C3 alkylcarbonyl such as acetyl and the like.

The term “cycloalkane” includes a monocyclic or polycyclic saturated cyclic carbocyclic ring containing from 3 to 10 carbons. Monocyclic cycloalkane includes, for example, cyclopropane, cyclobutane, cyclopentane, cyclohexane, cycloheptane, cyclooctane, cyclononane, cyclodecane, etc. Polycyclic cycloalkane includes norbornanane, tetrahydronaphthalene, etc.

Preferable “cycloalkane” for Ring A is C3-C6 monocyclic cycloalkane such as cyclohexane and the like.

The term “cycloalkyl” includes a monovalent group derived from “cycloalkane” as defined above.

Monocyclic cycloalkyl includes, for example, cyclopropyl, cyclobutyl, cyclopentyl, cyclohexyl, cycloheptyl, cyclooctyl, cyclononyl, cyclodecyl, etc. Polycyclic cycloalkyl includes norbornanyl, tetrahydronaphthalene-5-yl, tetrahydronaphthalene-6-yl, etc.

Preferable “cycloalkyl” for Ring R²is C3-C6 monocyclic cycloalkyl such as cyclopentyl, cyclohexyl, and the like.

The term “cycloalkane-diyl” includes a divalent group derived from “cycloalkane” as defined above. Monocyclic cycloalkane-diyl includes, for example, cyclopropane-diyl, cyclobutane-diyl, cyclopentane-diyl, cyclohexane-diyl, cycloheptane-diyl, cyclooctane-diyl, cyclonone-diyl, cyclodecane-diyl, etc. Polycyclic cycloalkane-diyl includes norbornane-diyl, etc.

Preferable “cycloalkane-diyl” for B is C3-C6 monocyclic cycloalkane-diyl such as cyclopentane-diyl, cyclohexane-diyl, and the like.

The term “cycloalkene” includes a non-aromatic monocyclic or polycyclic ring of 3 to 10 carbons containing at least one carbon-carbon double bond. Monocyclic cycloalkene includes, for example, cyclopentene, cyclohexene, etc. Polycyclic cycloalkene includes norborne, indene, etc.

The term “cycloalkenyl” includes a monovalent group derived from “cycloalkene” as defined above. Monocyclic cycloalkenyl includes cyclopentenyl, cyclohexenyl, etc. Polycyclic cycloalkenyl includes norbornyl, indene-1-yl, indene-2-yl, indene-3-yl, etc.

The term “cycloalkene-diyl” includes a divalent group derived from “cycloalkene” as defined above. Monocyclic cycloalkene-diyl includes cyclopentene-diyl, cyclohexene-diyl, etc. Polycyclic cycloalkene-diyl includes norbornene-diyl, etc.

Preferable “cycloalkene-diyl” for B is C3-C6 monocyclic cycloalkene-diyl such as cyclopentene-diyl, cyclohexene-diyl, and the like.

The term “aromatic carbocyclic ring” includes an aromatic hydrocarbocyclic ring which is monocyclic or fused-cyclic, such as benzene ring, naphthalene ring, anthracene ring, phenanthrene ring, etc.

Benzene ring is preferable as “aromatic carbocyclic ring” for ring A.

The term “aryl” includes a monovalent group derived from “aromatic carbocyclic ring” as defined above. For example, phenyl, 1-naphthyl, 2-naphthyl, anthryl, phenanthryl, etc. are exemplified.

Preferable “aryl” for R³is phenyl.

The term “aromatic carbocyclic ring-diyl” includes a divalent group derived from “aromatic carbocyclic ring” as defined above. For example, 1,2-phenylene, 1,3-phenylene, 1,4-phenylene, 1,2-naphthalene etc.

Preferable “aromatic carbocyclic ring-diyl” for B is 1,2-phenylene, 1,3-phenylene, 1,4-phenylene, and the like. More preferably, 1,4-phenylene and the like are exemplified.

The term “heterocyclic ring” includes an aromatic or a non-aromatic monocyclic or fused-cyclic ring, which includes a five- to seven-membered ring having at least one nitrogen atom, oxygen atom, and/or sulphur atom in the ring; a fused ring consisting of two or more said five- to seven-membered rings; or a fused ring consisting of said five- to seven-membered ring having at least one nitrogen atom, oxygen atom, and/or sulphur atom in the ring fused to one or more “aromatic carbocyclic ring”,“cycloalkane” or “cycloalkene” as defined above.

For example, a non-aromatic heterocyclic ring such as pyrroline, pyrrolidine, imidazole, pyrazole, piperidine, piperazine, morpholine, thiomorpholine, tetrahydropyrane, dihydropyridine, dihydropyridazine, dioxane, oxathiolane, thiane, tetrahydrofuran, tetrahydropyran, tetrahydrothiazole, tetrahydroisothiazole, etc.;

a monocyclic aromatic heterocyclic ring such as pyrrole, pyrazine, pyrazole, tetrazole, furan, thiophene, pyridine, imidazole, triazole, tetrazole, triazine, pyridazine, pyrimidine, isoxazole, thiazole, isothiazole, thiadiazole, oxazole, oxadiazole, etc; and

a fused heterocyclic ring such as indole, isoindole, indazole, indolizine, indoline, isoindoline, quinoline, isoquinoline, cinnoline, phthalazine, quinazoline, naphthyridine, quinoxaline, purine, pteridine, benzopyrane, benzimidazole, benzisoxazole, benzoxazole, benzoxadiazole, benzisothiazole, benzothiazole, benzothiadiazole, benzofuran, isobenzofuran, benzothiophene, benzotriazole, imidazopyridine, triazolopyridine, imidazothiazole, pyrazinopyridazine, benzimidazole, benzodioxane, tetrahydroquinoline, tetrahydrobenzothiophene, etc. are exemplified.

Preferable “heterocyclic ring” for Ring A is piperidine, thiophene, furan, pyridine, benzothiophene, benzothiazole, benzoxazole, and the like.

The term “heterocyclic group” includes a monovalent group derived from “heterocyclic ring” as defined above. For example, non-aromatic heterocyclic groups such as pyrrolinyl, pyrrolidino, pyrrolidinyl, imidazolynyl, imidazolidinyl, pyrazolinyl, pyrazolidinyl, piperidino, piperidyl, piperidino, piperazinyl, morpholinyl, morpholino, thiomorpholinyl, thiomorpholino, tetrahydropyranyl, dihydropyridyl, dihydropyridazinyl, dihydropyrazinyl, dioxanyl, oxathiolanyl, thianyl, tetrahydrofuryl, tetrahydropyranyl, tetrahydrothiazolinyl, tetrahydroisothiazolinyl, etc.;

monocyclic aromatic heterocyclic groups such as pyrrolyl, pyrazinyl, pyrazolyl, tetrazolyl, furyl, thienyl, pyridyl, imidazolyl, triazolyl, tetrazolyl, triazinyl, pyridazinyl, pyrimidinyl, pyrazinyl, isoxazolyl, thiazolyl, isothiazolyl, thiadiazolyl, oxazolyl and oxadiazolyl, etc; and

fused heterocyclic groups such as indolyl, isoindolyl, indazolyl, indolizinyl, indolinyl, isoindolinyl, quinolyl, isoquinolyl, cinnolinyl, phthalazinyl, quinazolinyl, naphthyridinyl, quinoxalinyl, purinyl, pteridinyl, benzopyranyl, benzimidazolyl, benzisoxazolyl, benzoxazolyl, benzoxadiazolyl, benzisothiazolyl, benzothiazolyl, benzothiadiazolyl, benzofuryl, isobenzofuryl, benzothienyl, benzotriazolyl, imidazopyridyl, triazolopyridyl, imidazothiazolyl, pyrazinopyridazinyl, benzimidazolynyl, benzodioxanyl, tetrahydroquinoline, tetrahydrobenzothienyl, etc. are exemplified.

Preferable “heterocyclic group” for Y is pyperidino, morpholino, and the like.

The term “heterocyclic ring-diyl” includes a divalent group derived from “heterocyclic ring” as defined above. For example, non-aromatic heterocyclic ring-diyl such as pyrrolin-diyl, pyrrolidin-diyl, imidazole-diyl, imidazolidin-diyl, pyrazolin-diyl, pyrazolidin-diyl, piperidin-diyl, piperazine-diyl, morpholin-diyl, thiomorpholin-diyl, tetrahydropyran-diyl, dihydropyridine-diyl, dihydropyridazin-diyl, dihydropyrazin-diyl, dioxan-diyl, oxathiolan-diyl, thian-diyl, tetrahydrofuran-diyl, tetrahydropyran-diyl, tetrahydrothiazol-diyl, tetrahydroisothiazol-diyl, etc.;

a monocyclic aromatic heterocyclic ring-diyl such as pyrrole-diyl, pyrazine-diyl, pyrazole-diyl, tetrazole-diyl, furan-diyl, thiophene-diyl, pyridine-diyl, imidazole-diyl, triazole-diyl, tetrazole-diyl, triazine-diyl, pyridazine-diyl, pyrimidine-diyl, pyrazine-diyl, isoxazole-diyl, thiazole-diyl, isothiazole-diyl, thiadiazole-diyl, oxazole-diyl, oxadiazole-diyl, etc; and

a fused heterocyclic ring-diyl such as indole-diyl, isoindole-diyl, indazole-diyl, indolizine-diyl, indoline-diyl, isoindoline-diyl, quinoline-diyl, isoquinoline-diyl, cinnoline-diyl, phthalazine-diyl, quinazoline-diyl, naphthyridine-diyl, quinoxaline-diyl, purine-diyl, pteridine-diyl, benzopyrane-diyl, benzimidazole-diyl, benzisoxazole-diyl, benzoxazole-diyl, benzoxadiazole-diyl, benzisothiazole-diyl, benzothiazole-diyl, benzothiadiazole-diyl, benzofuran-diyl, isobenzofuran-diyl, benzothiophene-diyl, benzotriazole-diyl, imidazopyridine-diyl, triazolopyridine-diyl, imidazothiazole-diyl, pyrazinopyridazine-diyl, benzimidazole-diyl, benzodioxane-diyl, tetrahydroquinoline-diyl, tetrahydrobenzothiophene-diyl, etc. are exemplified.

Preferable “heterocyclic ring-diyl” for B is pyrole-diyl, pyrazine-diyl, pyrazole-diyl, tetrazole-diyl, furan-diyl, thiophene-diyl, pyridine-diyl, imidazole-diyl, triazole-diyl, tetrazole-diyl, triazine-diyl, pyridazine-diyl, pyrimidine-diyl, pyrazine-diyl, isoxazole-diyl, thiazole-diyl, isothiazole-diyl, thiadiazole-diyl, oxazole-diyl, oxadiazole-diyl, and the like.

More preferably, dihydrothiazole-diyl, pyroridine-diyl, thiazole-diyl, thiophene-diyl, pyrrol-diyl, furan-diyl, isoxazole-diyl, thiadiazole-diyl, and the like are exemplified.

The term “non-aromatic carbocyclic ring” includes “cycloalkane” as defined above, “cycloalkene” as defined above, a fused ring consisting of “aromatic carbocyclic ring” as defined above fused to “cycloalkane” as defined above, and a fused ring consisting of “aromatic carbocyclic ring” as defined above fused to “cycloalkene” as defined above. As a fused ring, indene and the like are exemplified.

The term “aromatic heterocyclic ring” includes aromatic rings of “heterocyclic ring” as defined above. “Aromatic heterocyclic ring” includes a five- to seven-membered aromatic ring having at least one nitrogen atom, oxygen atom, and/or sulphur atom in the ring; a fused aromatic ring consisting of two or more said rings; and a fused ring consisting of a five- to seven-membered aromatic ring having at least one nitrogen atom, oxygen atom, and/or sulphur atom in the ring fused to one or more “aromatic carbocyclic ring” as defined above.

For example, a monocyclic aromatic heterocyclic ring such as pyrazine, pyrazole, tetrazole, furan, thiophene, pyridine, imidazole, triazole, triazine, pyridazine, pyrimidine, pyrazine, isoxazole, thiazole, isothiazole, thiadiazole, oxazole, oxadiazole, etc; and

a fused aromatic heterocyclic ring such as indole, isoindole, indazole, indolizine, quinoline, isoquinoline, cinnoline, phthalazine, quinazoline, naphthyridine, quinoxaline, purine, pteridine, benzimidazole, benzisoxazole, benzoxazole, benzoxadiazole, benzisothiazole, benzothiazole, benzothiadiazole, benzofuran, isobenzofuran, benzothiophene, benzotriazole, imidazopyridine, triazolopyridine, imidazothiazole, pyrazinopyridazine, benzimidazoline, etc. are exemplified.

The term “heteroaryl” includes a monovalent group derived from “aromatic heterocyclic ring” as defined above. “Heteroaryl” includes a five- to seven-membered aromatic group having at least one nitrogen atom, oxygen atom, and/or sulphur atom in the ring; a fused aromatic group consisting of two or more said rings; and a fused ring consisting of a five- to seven-membered aromatic group having at least one nitrogen atom, oxygen atom, and/or sulphur atom in the ring fused to one or more “aromatic carbocyclic ring” as defined above.

For example, monocyclic aromatic heterocyclic groups such as pyrrolyl, pyrazinyl, pyrazolyl, tetrazolyl, furyl, thienyl, pyridyl, imidazolyl, triazolyl, tetrazolyl, triazinyl, pyridazinyl, pyrimidinyl, pyrazinyl, isoxazolyl, thiazolyl, isothiazolyl, thiadiazolyl, oxazolyl, oxadiazolyl, etc; and

fused heterocyclic aromatic groups such as indolyl, isoindolyl, indazolyl, indolizinyl, isoindolinyl, quinolyl, isoquinolyl, cinnolinyl, phthalazinyl, quinazolinyl, naphthyridinyl, quinoxalinyl, purinyl, pteridinyl, benzimidazolyl, benzisoxazolyl, benzoxazolyl, benzoxadiazolyl, benzisothiazolyl, benzothiazolyl, benzothiadiazolyl, benzofuryl, isobenzofuryl, benzothienyl, benzotriazolyl, imidazopyridyl, triazolopyridyl, imidazothiazolyl, pyrazinopyridazinyl, benzimidazolynyl, etc. are exemplified.

The term “non-Aromatic heterocyclic ring” includes non-aromatic rings of “heterocyclic ring” as defined above. “Non-aromatic heterocyclic ring” includes, a five- to seven-membered non-aromatic ring having at least one nitrogen atom, oxygen atom, and/or sulphur atom in the ring; a fused non-aromatic ring consisting of two or more said rings; a fused ring consisting of a five- to seven-membered aromatic ring having at least one nitrogen atom, oxygen atom, and/or sulphur atom in the ring fused to one or more “cycloalkane” as defined above or “cycloalkene” as defined above; or a fused ring consisting of a five- to seven-membered non-aromatic heterocyclic ring having at least one nitrogen atom, oxygen atom, and/or sulphur atom in the ring fused to one or more “aromatic carbocyclic ring” as defined above or “non-aromatic carbocyclic ring” as defined above

For example, non-aromatic heterocyclic ring such as pyrroline, pyrrolidine, imidazoline, imidazolidine, pyrazoline, pyrazolidine, piperidine, piperazine, morpholine, thiomorpholine, thiomorpholine, tetrahydropyrane, dihydropyridine, dihydropyridazine, dihydropyrazine, dioxane, oxathiolane, thiane, tetrahydrofuran, tetrahydropyran, tetrahydrothiazolin, tetrahydroisothiazole, etc.;

a fused non-aromatic heterocyclic ring such as indoline, isoindoline, benzopyrane, benzodioxane, tetrahydroquinoline, tetrahydrobenzothiophene, etc. are exemplified.

The term “halogen” means fluorine, chlorine, bromine and iodine.

The term “lower alkoxy” includes a group of the formula RO— wherein R is as defined above for lower alkyl, such as methoxy, ethoxy, propoxy, isopropoxy, butoxy, isobutoxy, sec-butoxy, tert-butoxy, pentoxy, isopentoxy, neopentoxy, hexoxy, etc.

Preferable “lower alkoxy” for Y is C1-C4 alkoxy such as methoxy, ethoxy, propoxy, isopropoxy, butoxy, and the like.

The term “lower alkylthio” includes a group of the formula RS— wherein R is as defined above for lower alkyl, such as methylthio, ethylthio, propylthio, isopropylthio, butylthio, isobutylthio, sec-butylthio, tert-butylthio, pentylthio, isopentylthio, neopentylthio, hexylthio, etc.

Preferable “lower alkylthio” for R^1ais C1-C4 alkylthio such as methylthio and the like.

The term “lower alkoxycarbonyl” includes a group of the formula R—O—C(═O)— wherein R is as defined above for lower alkyl, such as methyloxycarbonyl, ethyloxycarbonyl, n-propyloxycarbonyl, isopropyloxycarbonyl, n-butyloxycarbonyl, tert-butyloxycarbonyl, n-pentyloxycarbonyl, etc.

Preferable “lower alkoxycarbonyl” for R^1a, R³and Y is C1-C4 alkoxycarbonyl such as methyloxycarbonyl, ethyloxycarbonyl, and the like.

The term “lower alkylcarbamoyl” includes mono- or di-lower alkylcarbamoyl wherein alkyl moiety contains from 1 to 6 carbons, such as methylcarbamoyl, ethylcarbamoyl, n-propylcarbamoyl, isopropylcarbamoyl, n-butylcarbamoyl, dimethylcarbamoyl, diethylcarbamoyl, dipropylcarbamoyl, etc.

Preferable “lower alkylcarbamoyl” for R^1ais C1-C4 alkoxycarbamoyl such as methylcarbamoyl, dimethylcarbamoyl, and the like.

The term “thiocarbamoyl” includes a group of the formula —C(═S)—NR^XR^Ywherein R^Xand R^Yare each independently hydrogen, “alkyl” or “alkenyl” as defined above, or “aryl”, “heteroaryl”, “non-aromatic carbocyclic group”, non-aromatic heterocyclic group”, “arylalkyl” or “heteroaryl alkyl” as defined below, and these are optionally and independently substituted with hydroxy, carboxy, “alkyl”, “alkenyl”, “alkynyl”, “halogen”, “alkyloxy”, “alkenyloxy”, “alkynyloxy”, “alkylthio”, “carbamoyl”, “alkyloxycarbonyl”, “aryloxycarbonyl” as defined above or below, and the like.

The term “sulfinyl” includes a group of the formula —S(═O)—R wherein R is “alkyl” or “alkenyl” as defined above, or “aryl”, “heteroaryl”, “non-aromatic carbocyclic group”, non-aromatic heterocyclic group”, “arylalkyl” or “heteroaryl alkyl” as defined below, and these are optionally and independently substituted with hydroxy, carboxy, “alkyl”, “alkenyl”, “alkynyl”, “halogen”, “alkyloxy”, “alkenyloxy”, “alkynyloxy”, “alkylthio”, “carbamoyl”, “alkyloxycarbonyl”, “aryloxycarbonyl” as defined above or below, and the like.

Preferable “sulfinyl” for R^1aand Y is C1-C4 alkylsulfinyl such as methylsulfinyl, and the like.

The term “sulfonyl” includes a group of the formula —S(═O)₂—R wherein R is “alkyl” or “alkenyl” as defined above, or “aryl”, “heteroaryl”, “non-aromatic carbocyclic group”, non-aromatic heterocyclic group”, “arylalkyl” or “heteroaryl alkyl” as defined below, and these are optionally and independently substituted with hydroxy, carboxy, “alkyl”, “alkenyl”, “alkynyl”, “halogen”, “alkyloxy”, “alkenyloxy”, “alkynyloxy”, “alkylthio”, “carbamoyl”, “alkyloxycarbonyl”, “aryloxycarbonyl” as defined above or below, and the like.

Preferable “sulfonyl” for R^1aand Y is C1-C4 alkylsulfonyl such as methylsulfonyl, and the like.

The term “sulfamoyl” includes a group of the formula —S(═O)₂—NR^XR^Ywherein R^Xand R^Yare each independently hydrogen, “alkyl” or “alkenyl” as defined above, or “aryl”, “heteroaryl”, “non-aromatic carbocyclic group”, non-aromatic heterocyclic group”, “arylalkyl” or “heteroaryl alkyl” as defined below, and these are optionally and independently substituted with hydroxy, carboxy, “alkyl”, “alkenyl”, “alkynyl”, “halogen”, “alkyloxy”, “alkenyloxy”, “alkynyloxy”, “alkylthio”, “carbamoyl”, “alkyloxycarbonyl”, “aryloxycarbonyl” as defined above or below, and the like.

Substituents for “substituted lower alkyl”, “substituted tert-butyl”, “substituted i-propyl”, “substituted lower alkenyl”, “substituted lower alkynyl”, “substituted lower alkoxy”, “substituted lower alkylthio”, “substituted lower alkoxycarbonyl”, and “substituted lower alkylcarbamoyl” include but are not limited to one or more same or different substituents selected from the group consisting of:

hydroxy, carboxy, halogen (F, Cl, Br, I), lower haloalkoxy (e.g., CF₃O), cycloalkyl (e.g., cyclopropyl), cycloalkenyl (e.g., cyclopropenyl), lower alkoxy (e.g., methoxy, ethoxy, propoxy, butoxy, etc.), lower alkenyloxy (e.g., vinyloxy, allyloxy, etc.), lower alkoxycarbonyl (e.g., methoxycarbonyl, ethoxycarbonyl, tert-butoxycarbonyl, etc.), nitro, nitroso, amino, lower alkylamino (e.g., methylamino, ethylamino, dimethylamino, etc.), acylamino (e.g., acetylamino, benzoylamino, etc.), aralkylamino (e.g., benzylamino, tritylamino), hydroxyamino, imino, hydroxyimino, lower alkylimino (e.g., methylimino, ethylimino, dimethylimino, etc.), lower alkoxyimino (e.g., methoxyimino, ethoxyimino, etc.), acylimino (e.g., acetylimino, benzoylimino, etc.), azido, aryl (e.g., phenyl, etc.), aralkyl (e.g., benzyl, etc.), aralkyloxy (e.g., benzyloxy), cyano, isocyano, isocyanato, thiocyanato, isothiocyanato, mercapto, lower alkylthio (e.g., methylthio, etc.), lower alkylsulfonyl (e.g., methanesulfonyl, ethanesulfonyl), carbamoyl, lower alkylcarbamoyl (e.g., methylcarbamoyl, ethylcarbamoyl, dimethylcarbamoyl, etc.), sulfamoyl, lower alkylsulfamoyl, acyl (e.g., formyl, acetyl, etc.), formyloxy, thioformyl, thiocarboxy, dithiocarboxy, thiocarbamoyl, sulfino, sulfo, hydrazino, azido, ureido, amidino, guanidino, phthalimido, tri-lower alkylsilyl (e.g., trimethylsilyl, etc.), and oxo.

Preferable substituents for “substituted lower alkyl” of R^1aand R^1bare hydroxy, halogen, nitro, cyano, lower haloalkoxy, lower alkenyloxy and the like. More preferable substituents are hydroxy, lower alkoxy and the like.

Preferable substituents for “substituted lower alkoxy” and “substituted lower alkylthio” of R^1aand R^1bare halogen, hydroxy and the like.

Preferable substituents for “substituted lower alkyl” Y are hydroxy, halogen, cyano, carboxy, carbamoyl, lower alkoxy, lower haloalkoxy, lower alkylcarbamoyl, amino, lower alkylamino, amino substituted with lower alkylsulfonyl, lower alkyloxycarbonylmethyloxy and the like.

More preferable substituents are hydroxy, halogen, cyano carboxy, carbamoyl, lower alkoxy, lower alkylcarbamoyl, amino, lower alkylamino, amino substituted with lower alkylsulfonyl, lower alkyloxycarbonylmethyloxy and the like.

Preferable substituents for “substituted lower alkoxy” and “substituted lower alkylthio” of Y are halogen, carboxy, cyano, hydroxy, lower alkyl, lower alkyl substituted with hydroxy, lower alkoxy, lower haloalkoxy, lower alkenyloxy, lower alkoxycarbonyl, amino, lower alkylamino, amino substituted with lower alkylsulfonyl, lower alkylsulfinyl, lower alkylsulfonyl, carbamoyl, lower alkylcarbamoyl, carbamoyl substituted with amino, carbamoyl substituted with hydroxy, lower alkylsulfinyl, lower alkylsulfonyl, cycloalkyl, a heterocyclic group and the like.

More preferable substituents are halogen, carboxy, cyano, carbamoyl, lower alkylcarbamoyl, imino substituted with hydroxy, lower alkoxy, amino, lower alkylamino, lower alkoxycarbonyl, lower alkylsulfinyl, tetrazolyl and the like.

Substituents for “substituted acyl” are as defined above for “substituted lower alkyl”. If R in acyl (R—C(═O)—) is “aryl”, “a heterocyclic group”, “cycloalkyl” or “cycloalkenyl”, then each ring may be substituted with lower alkyl (e.g., methyl, ethyl, isopropyl, tert-butyl, etc.), lower haloalkyl (e.g., CF₃, CH₂CF₃, CH₂CCl₃, etc.), lower alkenyl, lower alkynyl (e.g., ethynyl), etc.

Substituents for “substituted carbamoyl”, “substituted thiocarbamoyl” and “substituted sulfamoyl” are one or more same or different groups selected from, but are not limited to, the group consisting of:

hydroxy, carboxy, halogen (F, Cl, Br, I), lower alkyl (e.g., methyl), lower alkenyl (e.g., vinyl), lower alkynyl (e.g., ethynyl), cycloalkyl (e.g., cyclopropyl), cycloalkenyl (e.g., cyclopropenyl), lower alkoxycarbonyl (e.g., methoxycarbonyl, ethoxycarbonyl, tert-butoxycarbonyl, etc.), amino, lower alkylamino (e.g., methylamino, ethylamino, dimethylamino, etc.), acylamino (e.g., acetylamino, benzoylamino, etc.), aralkylamino (e.g., benzylamino, tritylamino), hydroxyamino, aryl (e.g., phenyl, etc.), cyano, isocyano, isocyanato, thiocyanato, isothiocyanato and acyl (e.g., formyl, acetyl, etc.).

Preferable substituents for “substituted carbamoyl”, “substituted thiocarbamoyl” and “substituted sulfamoyl” of R^1aand R^1bare lower alkyl, lower alkenyl, lower alkynyl, amino, lower alkylamino, acyl amino, hydroxy amino and the like.

More preferable substituents are lower alkyl, lower alkylamino and the like.

Preferable substituents for “substituted carbamoyl” of Y are lower alkyl, lower alkyl substituted with hydroxy, lower alkyl substituted with lower alkoxy, lower alkyl substituted with cyano, lower alkenyl, lower alkynyl, lower alkylamino, acyl amino and the like.

More preferable substituents are lower alkyl, lower alkyl substituted with hydroxy, lower alkyl substituted with lower alkoxy, lower alkyl substituted with cyano, lower alkylamino and the like.

Substituents for “substituted amino” are one or more same or different groups selected from, but are not limited to, the group consisting of:

hydroxy, halogen (F, Cl, Br, I), lower haloalkyl (e.g., CF₃, CH₂CF₃, CH₂CCl₃, etc.), hydroxy(lower)alkyl (e.g., hydroxyethyl, —C(CH₃)₂CH₂OH, etc.), lower haloalkoxy (e.g., CF₃O), lower alkyl (e.g., methyl, ethyl, isopropyl, tert-butyl, etc.), lower alkenyl (e.g., vinyl), lower alkynyl (e.g., ethynyl), cycloalkyl (e.g., cyclopropyl), cycloalkenyl (e.g., cyclopropenyl), lower alkoxy (e.g., methoxy, ethoxy, propoxy, butoxy, etc.), lower alkyloxycarbonyl (tert-butyloxycarbonyl, etc.), lower alkenyloxy (e.g., vinyloxy, allyloxy, etc.), amino, lower alkylamino (e.g., methylamino, ethylamino, dimethylamino, etc.), acylamino (e.g., acetylamino, benzoylamino, etc.), aralkylamino (e.g., benzylamino, tritylamino), hydroxyamino, imino, hydroxyimino, lower alkylimino (e.g., methylimino, ethylimino, dimethylimino, etc.), lower alkoxyimino (e.g., methoxyimino, ethoxyimino, etc.), acylimino (e.g., acetylimino, benzoylimino, etc.), aryl (e.g., phenyl, etc.), aralkyl (e.g., benzyl, etc.), cyano and acyl (e.g., formyl, acetyl, etc.).

Preferable substituents for “substituted amino” of R^1aand R^1bare lower alkyl, lower alkenyl, lower alkynyl, lower haloalkyl, lower hydroxyalkyl, lower alkoxy, lower haloalkoxy, lower alkenyloxy, acyl and the like.

More preferable substituents are lower alkyl, acyl and the like.

Preferable substituents for “substituted amino” of Y are lower alkyl, acetyl, lower alkyloxycarbonyl, carbamoyl, lower alkylsulfonyl and the like.

Substituents for “substituted cycloalkyl”, “substituted cycloalkenyl”, “substituted aryl”, “a substituted heterocyclic group”, “substituted heteroaryl”, “substituted phenyl”, and “substituted pyridyl” are one or more same or different groups selected from, but are not limited to, the group consisting of:

hydroxy, carboxy, halogen (F, Cl, Br, I), lower haloalkyl (e.g., CF₃, CH₂CF₃, CH₂CCl₃, etc.), lower haloalkoxy (e.g., CF₃O), lower alkyl (e.g., methyl, ethyl, isopropyl, tert-butyl, etc.), lower alkenyl (e.g., vinyl), lower alkynyl (e.g., ethynyl), cycloalkyl (e.g., cyclopropyl), cycloalkenyl (e.g., cyclopropenyl), lower alkoxy (e.g., methoxy, ethoxy, propoxy, butoxy, etc.), lower alkenyloxy (e.g., vinyloxy, allyloxy, etc.), lower alkoxycarbonyl (e.g., methoxycarbonyl, ethoxycarbonyl, tert-butoxycarbonyl, etc.), nitro, nitroso, amino, lower alkylamino (e.g., methylamino, ethylamino, dimethylamino, etc.), acylamino (e.g., acetylamino, benzoylamino, etc.), aralkylamino (e.g., benzylamino, tritylamino), hydroxyamino, imino, hydroxyimino, lower alkylimino (e.g., methylimino, ethylimino, dimethylimino, etc.), lower alkoxyimino (e.g., methoxyimino, ethoxyimino, etc.), acylimino (e.g., acetylimino, benzoylimino, etc.), azido, aryl (e.g., phenyl, etc.), aralkyl (e.g., benzyl, etc.), aralkyloxy (e.g., benzyloxy, etc.), cyano, isocyano, isocyanato, thiocyanato, isothiocyanato, mercapto, lower alkylthio (e.g., methylthio, etc.), lower alkylsulfonyl (e.g., methanesulfonyl, ethanesulfonyl), substituted or unsubstituted carbamoyl (e.g., carbamoyl, N-methyl-N-methoxycarbamoyl, etc.), substituted or unsubstituted lower alkylcarbamoyl (e.g., methylcarbamoyl, ethylcarbamoyl, dimethylcarbamoyl, hydroxy ethylcarbamoyl, trifluoromethylcarbamoyl, trifluoro ethylcarbamoyl, etc.), sulfamoyl, lower alkylsulfamoyl, acyl (e.g., formyl, acetyl, etc.), formyloxy, thioformyl, thiocarboxy, dithiocarboxy, thiocarbamoyl, sulfino, sulfo, hydrazino, azido, ureido, amidino, guanidino, phthalimido and oxo.

Preferable substituents for “substituted cycloalkyl”, “substituted cycloalkenyl”, “substituted aryl”, “a substituted heterocyclic group”, “substituted heteroaryl”, “substituted phenyl”, and “substituted pyridyl” are halogen, lower alkyl, lower haloalkyl, lower alkoxy, lower haloalkoxy and the like.

The halogen moiety in said “lower haloalkyl” and “lower haloalkoxy” is as defined above for “halogen”.

The alkyl or lower alkyl moiety in said “lower haloalkyl”, “lower alkylamino”, “lower alkylimino”, “lower alkylsulfonyl”, “lower alkylsulfamoyl”, “lower alkylcarbamoyl”, “aralkyl” and “aralkylamino” is as defined above for “lower alkyl”.

The lower alkoxy moiety of said “lower haloalkoxy” and “lower alkoxyimino” is as defined above for “lower alkoxy”.

The term “lower alkenyl” includes a straight or branched chain alkenyl containing from 2 to 6 carbons, preferably containing from 2 to 3 carbons, having one or more double bonds at any position. For example, vinyl, propenyl, isopropenyl, butenyl, isobutenyl, prenyl, butadienyl, pentenyl, isopentenyl, pentadienyl, hexenyl, isohexenyl, hexadienyl, etc. are exemplified.

The lower alkenyl moiety of “lower alkenyloxy” is as defined above for “lower alkenyl”.

The term “lower alkynyl” includes a straight or branched chain alkynyl containing from 2 to 6 carbons, preferably containing from 2 to 3 carbons. For example, ethynyl, propynyl, butynyl, pentynyl, hexynyl, etc. are exemplified. They have one or more triple bonds at any position, and optionally, have a double bond.

The term “aralkyl” includes a group “lower alkyl” as defined above substituted with above “aryl” as defined above. For example, benzyl, phenethyl and the like are exemplified.

The aryl moiety of “aralkylamino” and “aralkyl” is as defined above for “aryl”.

The acyl moiety of “acyl”, “acylamino” and “acylimino” is as defined above for “acyl”.

The protecting groups for “hydroxy optionally protected” and “mercapto optionally protected” are well known in the art and include for example, a group that forms ether and substituted ether, such as methyl, methoxymethyl, t-butoxymethyl, 1-ethoxyethyl and benzyl, etc.; a group that forms silyl ether, such as trimethylsilyl, triethylsilyl, tert-butyldimethylsilyl and methyldiisopropylsilyl; a group that forms ester, such as formate, acetate and trichloroacetate, etc.; a group that forms carbonate, such as methyl carbonate, 2,2,2-trichloroethyl carbonate, and p-nitrophenyl carbonate, etc.; a group that forms sulfonyl, such as methanesulfonyl, p-toluenesulfonyl, etc.

Preferable protective groups for “optionally protected hydroxy” and “optionally protected mercapto” are ether, a group that forms substituted ether and the like. More preferable are a group formed by substituted ether and the like.

In addition, one or more hydrogen, carbon or other atoms of a compound of Formula (I) can be replaced by an isotope of the hydrogen, carbon or other atoms. Compounds of Formula (I) include all radiolabeled forms of compounds of Formula (I) “radiolabeled,” “radiolabeled form”, and the like of a compound of Formula I, each of which is encompassed by the invention, is useful as a research and/or diagnostic tool in metabolism pharmacokinetic studies and in binding assays. Examples of isotopes that can be incorporated into a compound of Formula (I) of the invention include isotopes of hydrogen, carbon, nitrogen, oxygen, phosphorous, sulfur, fluorine and chlorine, such as ²H, ³H, ¹³C, ¹⁴C, ¹⁵N, ¹⁸O, ¹⁷O, ³¹P, ³²P, ³⁵S, ¹⁸P, and ³⁶Cl, respectively. Radiolabeled compounds of the invention can be prepared by methods known in the art. For example, tritiated compounds of Formula (I) can be prepared by introducing tritium into the particular compound of Formula (I), for example, by catalytic dehalogenation with tritium. This method may include reacting a suitably halogen-substituted precursor of a compound of Formula (I) with tritium gas in the presence of a suitable catalyst, for example, Pd/C, in the presence or absence of a base. Other suitable methods for preparing tritiated compounds can be found in Filer, “The Preparation and Characterization of Tritiated Neurochemicals,” Chapter 6, pp. 155-192 in Isotopes in the Physical and Biomedical Sciences, Vol. 1, Labeled Compounds (Part A) (1987). ¹⁴C-labeled compounds can be prepared by employing starting materials having a ¹⁴C carbon.

Preferred embodiments of the compound (I′) of the invention are as follows. Each variant is as defined above.

Z¹′ is hydroxy.

Z²′ is O.

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Ring A′ is an aromatic carbocyclic ring or a heterocyclic ring.

For example, an aromatic carbocyclic ring and an aromatic heterocyclic ring are exemplified as A′.

For example, benzene ring and pyridine ring are exemplified as Ring A′.

R²′ is substituted or unsubstituted aryl, or a substituted or unsubstituted aromatic heterocyclic group (e.g., thienyl, pyridyl, imidazolyl, pyrimidinyl, isoxazolyl, thiazolyl, isothiazolyl, thiadiazolyl, oxazolyl, pyrazolyl, oxadiazolyl, etc.).

For example, substituted or unsubstituted phenyl is exemplified as R²′.

For example, substituted or unsubstituted pyridyl is exemplified as R²′.

For example, substituted or unsubstituted tert-butyl is exemplified as R²′.

R³′ is substituted or unsubstituted alkyl, substituted or unsubstituted cycloalkyl, or substituted or unsubstituted phenyl.

For example, substituted or unsubstituted alkyl, substituted or unsubstituted cycloalkyl, substituted or unsubstituted aryl and substituted or an unsubstituted heterocyclic group are exemplified as R³′.

For example, a group represented by the following formula:

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are exemplified as R³′.

Ring D′ is benzene ring or pyridine ring.

V′ is “—O—C(═O)—”, “—C(═O)—O—”, “—NR¹³′—C(═O)—” or “—C(═O)—NR¹³′—”.

R^4a′ and R^4b′ are each independently hydrogen or lower alkyl.

For example, hydrogen is exemplified as R^4a′ and R^4b′.

t′ is 0.

m′ is an integer of 0 to 2.

For example, m′ is 1 or 2.

For example, m′ is 0.

R^1a′ is halogen, substituted or unsubstituted lower alkyl, carboxy, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted aryl or a substituted or unsubstituted heterocyclic group.

For example, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted phenyl, and a substituted or unsubstituted aromatic heterocyclic group (e.g., thienyl, pyridyl, imidazolyl, pyrimidinyl, isoxazolyl, thiazolyl, isothiazolyl, thiadiazolyl, oxazolyl, pyrazolyl, oxadiazolyl, etc.) are exemplified as R^1a′.

For example, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted aryl and a substituted or unsubstituted heterocyclic group are exemplified as R^1a′.

For example, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted phenyl, a substituted or unsubstituted aromatic heterocyclic group (e.g., thienyl, pyridyl, imidazolyl, pyrimidinyl, isoxazolyl, thiazolyl, isothiazolyl, thiadiazolyl, oxazolyl, pyrazolyl, oxadiazolyl, etc.) are exemplified as R^1a′.

R^1b′ is halogen, substituted or unsubstituted lower alkyl, carboxy, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted aryl or a substituted or unsubstituted heterocyclic group.

For example, halogen, substituted or unsubstituted lower alkyl, carboxy, and substituted or unsubstituted lower alkoxycarbonyl are exemplified as R^1b′.

Further, a compound represented by all combination of alternatives in each substituent as defined above is preferable.

Preferable embodiments of the compound (I′) of the present invention are as follows.

A compound wherein

Z²is O;

t is 0;

R²′ is substituted or unsubstituted tert-butyl, or substituted or unsubstituted i-propyl; and

R³is a group represented by the formula:

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A compound wherein

Z²′ is O;

t′ is 0; and

R²is a group represented by the formula:

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R³′ is substituted or unsubstituted aryl or a substituted or unsubstituted heterocyclic group.

A compound wherein

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t′ is 0;

R²′ is substituted or unsubstituted tert-butyl, or substituted or unsubstituted i-propyl; and

R³′ is a group represented by the formula:

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Further, a compound represented by all combination of alternatives in each substituent as defined above is preferable.

Preferable embodiments of the compound (I) of the present invention are as follows. Each variant is as defined above.

R²is a group represented by the formula:

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wherein Me is methyl and q is an integer of 0 to 4.

For example, a group represented by the formula:

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wherein Me is methyl and q is an integer of 0 to 1 as R².

R³is a group represented by the formula:

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For example, a group represented by the formula:

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are exemplified as R³.

For example, a group represented by the formula:

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are exemplified as R³.

For example, a group represented by the formula:

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are exemplified as R³.

Y is hydroxy, halogen, cyano, carboxy, substituted or unsubstituted lower alkyl, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted acyl, substituted or unsubstituted carbamoyl, substituted or unsubstituted thiocarbamoyl, substituted or unsubstituted lower alkylthio, substituted or unsubstituted lower alkylsulfamoyl, substituted or unsubstituted amino, substituted sulfinyl, substituted sulfonyl, or a substituted or unsubstituted heterocyclic group.

For example, substituted or unsubstituted lower alkyl, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted acyl, substituted or unsubstituted carbamoyl, substituted or unsubstituted thiocarbamoyl, substituted or unsubstituted lower alkylthio, substituted or unsubstituted lower alkylsulfamoyl, substituted or unsubstituted amino, substituted sulfinyl and substituted sulfonyl are exemplified as Y.

R¹⁴is halogen, hydroxy, substituted or unsubstituted lower alkyl, substituted or unsubstituted lower alkenyl, substituted or unsubstituted lower alkynyl, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkylthio, substituted or unsubstituted acyl, carboxy, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted carbamoyl, substituted or unsubstituted amino, substituted or unsubstituted sulfamoyl, cyano or nitro.

For example, halogen, hydroxy, substituted or unsubstituted lower alkyl, substituted or unsubstituted lower alkenyl, substituted or unsubstituted lower alkynyl, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkylthio, substituted or unsubstituted acyl, carboxy, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted carbamoyl, substituted or unsubstituted amino, substituted or unsubstituted sulfamoyl, cyano and nitro are exemplified as R¹⁴.

r is an integer of 0 to 2.

Further, a compound represented by all combination of alternatives in each substituent as defined above is preferable.

Further, more preferable embodiments of the compound (I) of the present invention are as follows.

(a) A compound wherein

R²is a group represented by the formula:

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wherein Me is methyl and q is an integer of 0 to 1; and

R³is a group represented by the formula:

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r is an integer of 0 to 2;

provided that the compounds represented by the following formula:

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are excluded,

or its pharmaceutically acceptable salt, or a solvate thereof.

Further, more preferable embodiments of the compound (I) of the present invention are as follows.

(b) A compound wherein

R²is a group represented by the formula:

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wherein Me is methyl and q is an integer of 0 to 1; and

R³is a group represented by the formula:

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wherein Y is substituted or unsubstituted alkoxy, substituted or unsubstituted alkylthio, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted carbamoyl, substituted or unsubstituted lower alkylsulfamoyl, substituted or unsubstituted amino, cyano, carboxy, substituted sulfinyl, substituted sulfonyl, a substituted or unsubstituted heterocyclic group;

r is an integer of 0 to 2;

provided that the compounds represented by the following formula:

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are excluded,

or its pharmaceutically acceptable salt, or a solvate thereof.

Further, more preferable embodiments of the compound (I) of the present invention are as follows.

R²is a group represented by the formula:

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wherein Me is methyl and q is an integer of 0 to 1; and

R³is a group represented by the formula:

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r is 0

provided that the compounds represented by the following formula:

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are excluded,

or its pharmaceutically acceptable salt, or a solvate thereof.

Further, more preferable embodiments of the compound (I) of the present invention are as follows.

(d) A compound wherein

Z¹is hydroxy;

Z²is —C(═O)—;

Z^3aand Z^3bare taken together ═O;

R²is a group represented by the formula:

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wherein Me is methyl and q is an integer of 0 to 1;

R³is a group represented by the formula:

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r is 0;

t is 0;

k is an integer of 0 or 1;

m is an integer of 0 or 1;

n is an integer of 0 or 1;

R^1aand R^1bare each independently halogen, hydroxy, substituted or unsubstituted lower alkyl, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkylthio, substituted or unsubstituted acyl, carboxy, substituted or unsubstituted lower alkoxycarbonyl, substituted or unsubstituted carbamoyl, substituted or unsubstituted thiocarbamoyl, substituted or unsubstituted amino, substituted sulfinyl, substituted sulfonyl, substituted or unsubstituted sulfamoyl, cyano, nitro or —C(R^7a)═N—O—R^7b; and

R^7aand R^7bare each independently hydrogen or substituted or unsubstituted lower alkyl;

provided that the compounds represented by the following formula:

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are excluded,

or its pharmaceutically acceptable salt, or a solvate thereof.

Further, more preferable embodiments of the compound (I) of the present invention are as follows.

(e) A compound wherein

Z¹is hydroxy;

Z²is —C(═O)—;

Z^3aand Z^3bare taken together ═O;

Ring A is benzene or pyridine;

B is aromatic carbocyclic ring-diyl or aromatic heterocyclic ring-diyl;

R²is a group represented by the formula:

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wherein Me is methyl and q is an integer of 0 to 1;

R³is a group represented by the formula:

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wherein Y is substituted or unsubstituted lower alkyl, substituted or unsubstituted lower alkoxy, substituted or unsubstituted lower alkylthio, or substituted or unsubstituted amino; and

r is 0;

t is 0;

k is 1;

m is an integer of 0 or L

n is an integer of 0 or 1; and

R^1aand R^1bare each independently halogen, substituted or unsubstituted lower alkyl, substituted or unsubstituted lower alkoxy, or substituted or unsubstituted lower alkylthio

provided that the compounds represented by the following formula:

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are excluded,

or its pharmaceutically acceptable salt, or a solvate thereof.

Further, more preferable embodiments of the compound (I) of the present invention are as follows.

(f) A compound wherein

Z¹is hydroxy;

Z²is —C(═O)—;

Z^3aand Z^3bare taken together ═O;

Ring A is benzene or pyridine;

B is aromatic carbocyclic ring-diyl or aromatic heterocyclic ring-diyl;

R²is a group represented by the formula:

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wherein Me is methyl and q is an integer of 0 to 1;

R³is a group represented by the formula:

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wherein Y is substituted lower alkoxy, substituted lower alkylthio, or substituted amino; and

r is 0;

t is 0;

k is 1;

m is 0 or 1;

n is 0 or 1; and

R^1aand R^1bare each independently halogen, substituted or unsubstituted lower alkyl, substituted or unsubstituted lower alkoxy, or substituted or unsubstituted lower alkylthio;

provided that the compounds represented by the following formula:

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are excluded,

or its pharmaceutically acceptable salt, or a solvate thereof.

(g) A compound as defined in the above (a) to (f), wherein Y is lower alkoxy substituted with one or more substituents selected from Substituent group A (Substituent group A: hydroxy, carbamoyl, lower alkylcarbamoyl, imino substituted with hydroxy, lower alkoxy, amino, lower alkylamino, lower alkoxycarbonyl, lower alkylsulfinyl and lower alkylsulfonyl), or its pharmaceutically acceptable salt, or a solvate thereof.

(h) A compound as defined in the above (a) to (g), wherein the formula represented by the formula:

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is a formula represented by the formula:

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wherein each substituent is as defined in the above (a) to (e), or its pharmaceutically acceptable salt, or a solvate thereof.

General procedures for the synthesis of the compound of the invention are described bellow. Starting materials and reaction reagents used in such synthesis are commercially available or can be prepared according to methods well known in the art using compounds commercially available.

The compound (I) of the invention, i.e., the compound of the general formula (I) (compounds represented by other formulae also can be referred to as such manner), may be prepared via the routes as described bellow.

[Route 1]

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wherein, R¹³is substituted or unsubstituted lower alkyl; all other variables are as defined above.

As shown, the compound of the invention of the general formula (Ia) may be prepared by the reaction of compound (II), compound (III) and compound (IV) without solvent or in an appropriate solvent, in the presence or absence of acid.

In this reaction, compound (III) and compound (IV) may be used in an amount of one equivalent or more, preferably 1 to 3 equivalents, in respect of compound (II).

Acid that may be used includes acetic acid, para-toluenesulfonic acid, hydrochloric acid, etc.

Solvent that may be used includes aromatic hydrocarbons (e.g., toluene, benzene, xylene, etc.), saturated hydrocarbons (e.g., cyclohexane, hexanes, etc.), ethers (e.g., tetrahydrofuran, diethyl ether, dioxane, etc.) and mixture thereof.

The temperature for such reaction may be −10° C. to 160° C., preferably 20° C. to 120° C. Reaction time depends on the compound, such reaction may be conducted for 10 minutes to 80 hours.

Optionally, desired compound (Ia) thus obtained may be purified according to conventional methods (e.g., column chromatography, recrystallization, etc.).

[Route 2]

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wherein all variables are as defined above.

As shown, the compound of the invention represented by the general formula (Ia) may be prepared by the reaction of compound (II) and compound (V) without solvent or in an appropriate solvent, in the presence or absence of acid.

In this reaction, compound (V) can be used in an amount of one equivalent or more, preferably 1 to 3 equivalents, in respect of compound (II).

Acid that may be used includes acetic acid, para-toluenesulfonic acid, hydrochloric acid, etc.

The temperature for such reaction may be −10° C. to 160° C., preferably 20° C. to 120° C. Although reaction time depends on the compound, such reaction may be conducted for 10 minutes to 80 hours.

Optionally, desired compound (Ia) thus obtained may be purified according to conventional methods (e.g., column chromatography, recrystallization, etc.).

[Route 3]

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wherein, one of L and Q is dihydroxyborane, di(lower)alkylborane or di(lower)alkoxyborane and the other is halogen or —OSO₂(C_iF_2i+1) wherein i is an integer 1 to 4, and all other variants are as defined above.

As shown, the compound of the invention represented by the general formula (Ib) may be prepared by Suzuki coupling of compound (VI) with compound (VII) in an appropriate solvent, in the presence of a palladium catalyst and a base.

In this reaction, compound (VII) can be used in an amount of one equivalent or more, preferably 1 to 3 equivalents, in respect of compound (VI).

Base that may be used includes metal hydroxide (e.g., sodium hydroxide, potassium hydroxide, potassium phosphate, etc.), metal hydride (e.g., sodium hydride, lithium hydride, etc.), metal carbonate (e.g., sodium carbonate, potassium carbonate, cesium carbonate, etc.), etc. Such base can be used in an amount of one equivalent or more, preferably 1 to 5 equivalents, in respect of compound (VI).

Palladium catalyst that can be used includes tris(dibenzylideneacetone)dipalladium(0), palladium acetate (II), dichlorobis(triphenylphosphine)palladium (II) or tetrakis(triphenylphosphine)palladium(II), etc., and may be used in an amount of 0.001 equivalent or more, preferably 0.01 to 1 equivalent, in respect of compound (VI).

The temperature for such reaction may be −10° C. to 180° C., preferably 20° C. to 120° C., optionally under microwave radiation. Although reaction time depends on the compound, such reaction may be conducted for 10 minute to 80 hours.

Optionally, desired compound (Ib) thus obtained may be purified according to conventional methods (e.g., column chromatography, recrystallization, etc.).

[Route 4]

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wherein, one of L and M is trialkyltin (e.g., —SnBu₃, etc.) and the other is halogen or —OSO₂(C_iF_2i+1) wherein i is an integer 1 to 4 and all other variants are as defined above.

As shown, the compound of the invention represented by the general formula (Ib) may be prepared by Stille coupling of compound (VI) with compound (VIII) in an appropriate solvent in the presence of a catalyst.

In this reaction, compound (VIII) can be used in an amount of one equivalent or more, preferably 1 to 3 equivalents, in respect of compound (VI).

Catalyst can be used include tris(dibenzylideneacetone)dipalladium(0), palladium acetate (II), dichlorobis(triphenylphosphine)palladium(II) or tetrakis(triphenylphosphine)palladium(II), etc., and may be used in an amount of 0.001 equivalent or more, preferably 0.01 to 1 equivalent, in respect of compound (VI). Optionally, phosphine ligand such as tri-tert-butylphosphine, 2-(di-tert-butylphosphino)biphenyl, 2-(dicyclohexylphosphino)biphenyl, triphenylphosphine, tris(2-furyl)phosphine, etc. may be added in twice molar amounts in respect of the catalyst.

Optionally, desired compound (Ib) thus obtained may be purified according to conventional methods (e.g., column chromatography, recrystallization, etc.).

[Route 5]

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wherein all other variants are as defined above.

As shown, the compound of the invention represented by the general formula (X) may be prepared by the reaction of the compound (IX) in an appropriate solvent, in the presence of an oxidizing agent.

Oxidizing agent that may be used includes manganese dioxide, 2-iodoxybenzoic acid, etc., and may be used in an amount of one equivalent or more, preferably 1 to 1.5 equivalents, in respect of compound (IX).

Solvent that may be used includes aromatic hydrocarbons (e.g., toluene, benzene, xylene, etc.), saturated hydrocarbons (e.g., cyclohexane, hexanes, etc.), halogenated hydrocarbons (e.g., dichloromethane, 1,2-dichloroethane, etc.), ethers (e.g., tetrahydrofuran, dioxane, etc.), ketones (e.g., acetone, methylethyl ketone, etc.), nitriles (e.g., acetonitrile, etc.) and mixture thereof, etc.

The temperature for such reaction may be −10° C. to 150° C., preferably 20° C. to 100° C. Although reaction time depends on the compound, such reaction may be conducted for 10 minutes to 80 hours.

The compound (IX) obtained may be used in the next step as a crude product or after purification according to conventional methods (e.g., column chromatography, recrystallization, etc.).

[Route 5 (continued)]

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wherein, i is an integer 0 to 3; X¹and X²are independently NR¹⁴, O or S; R¹⁴is hydrogen or lower alkyl; all other variables are as defined above.

As shown, the compound of the invention represented by the general formula (Ic) may be prepared by the reaction of compound (X) and compound (XI) without solvent or in an appropriate solvent, in the presence or absence of an acid.

In this reaction, compound (XI) can be used in an amount of one equivalent or more, preferably 1 to 3 equivalents, in respect of compound (X).

Acid that may be used includes p-toluenesulfonic acid, sulfuric acid, p-toluenesulfonic acid pyridinium salt, etc.

Solvent that may be used includes aromatic hydrocarbons (e.g., toluene, benzene, xylene, etc.), saturated hydrocarbons (e.g., cyclohexane, hexanes, etc.), and mixture thereof.

The temperature for such reaction may be −10° C. to 170° C., preferably 20° C. to 150° C. Reaction time depends on the compound, such reaction may be conducted for 10 minutes to 80 hours.

Optionally, desired compound (Ic) thus obtained may be purified according to conventional methods (e.g., column chromatography, recrystallization, etc.).

[Route 6]

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wherein all variables are as defined above.

As shown, the compound of the invention represented by the general formula (Id) may be prepared by the reaction of compound (X) and compound (XII) or a salt thereof in an appropriate solvent. The compound (XII) or a salt thereof can be used in an amount of 1 to 4 equivalents, preferably 1 to 2.5 equivalents, in respect of compound (X).

Salts of compound (XII) include mineral acid salts such as hydrochloride, sulfate, etc. Such salt is neutralized with a base when it is used in the reaction.

Base that may be used includes sodium acetate, amines (pyridinium, etc.), etc., and can be used in an amount of 1 to 3 equivalents, preferably 1 to 2 equivalents, in respect of the salt of compound (XI).

Solvent that may be used includes aromatic hydrocarbons (e.g., toluene, benzene, xylene, etc.), halogenated hydrocarbons (e.g., chloroform, 1,2-dichloroethane, etc.), ethers (e.g., tetrahydrofuran, dioxane, etc.), alcohols (e.g., methanol, enthanol, n-propanol, iso-propanol, etc.), water and mixture thereof, etc.

Reaction temperature is 0° C. to 150° C., preferably 20° C. to 120° C.

Reaction time is generally from about 10 minutes to 24 hours.

Optionally, desired compound (Id) thus obtained may be purified according to conventional methods (e.g., column chromatography, recrystallization, etc.).

[Route 7]

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wherein, Hal is halogen; R⁹is a hydroxy protecting group; all other variables are as defined above.

As shown, the compound of the invention represented by the general formula (Ie) may be prepared by the reaction of the compound (Ia) and the compound (XIII) in an appropriate solvent in the presence of a base. The compound (XII) can be used in an amount of 1 to 4 equivalents, preferably 1 to 2.5 equivalents, in respect of compound (Ia).

Base that may be used includes sodium hydride, sodium methoxide, amines, etc. (triethylamine, pyridinium, etc.) and can be used in an amount of 1 to 3 equivalents, preferably 1 to 2 equivalents, in respect of the salt of compound (Ia).

Solvent that may be used includes aromatic hydrocarbons (e.g., toluene, benzene, xylene, etc.), halogenated hydrocarbons (e.g., chloroform, 1,2-dichloroethane, etc.), ethers (e.g., tetrahydrofuran, dioxane, etc.), N,N-dimethylformamide, dimethylsulfoxide and mixture thereof, etc.

Reaction temperature is −20° C. to 150° C., preferably 0° C. to 120° C.

Reaction time is generally from about 10 minutes to 24 hours.

Optionally, desired compound (Ie) thus obtained may be purified according to conventional methods (e.g., column chromatography, recrystallization, etc.).

[Route 8]

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wherein the variables are as defined above.

As shown, the compound of the invention represented by the general formula (Ih) may be prepared by the reaction of compound (Ia) and compound (XIV) in an appropriate solvent. The compound (XIV) can be used in an amount of 1 to 4 equivalents, preferably 1 to 2.5 equivalents, in respect of compound (Ia).

Solvent that may be used includes acetic acid, hydrocarbons (e.g., benzene, toluene, xylene, etc.), ethers (e.g., tetrahydrofuran, dioxane, etc.), alcohols (e.g., methanol, enthanol, n-propanol, isopropanol, etc.) and mixture thereof, etc.

Reaction temperature is 0° C. to 150° C., preferably 50° C. to 130° C.

Reaction time is generally from about 10 minutes to 24 hours.

Optionally, desired compound (Ih) thus obtained may be purified according to conventional methods (e.g., column chromatography, recrystallization, etc.).

[Route 9]

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wherein the variables are as defined above.

In this reaction, compound (II) and a reagent for optical resolution (XV) (e.g., (R) or (S)-methyl-2-hydroxy-2-phenylacetate) are reacted with a condensing agent (e.g., Diisopropyl Azodicarboxylate) in an appropriate solvent to give a mixture. The mixture is purified according to conventional methods (e.g., column chromatography, recrystallization, etc.) to isolate a diastereomer having a desired configuration. The obtained diastereomer is subjected to a deprotection reaction (e.g., hydrogenation, lithium chloride, etc.) to obtain a desired enantiomer. The reagent for optical resolution can be used in an amount of 1 to 4 equivalents, preferably 1 to 2.5 equivalents, in respect of compound (Ii).

Solvent that may be used includes aromatic hydrocarbons (e.g., toluene, benzene, xylene, etc.), saturated hydrocarbons (e.g., cyclohexane, hexane, 1,3-dimethyl-2-imidazolidinone, etc.), ethers (e.g., tetrahydrofuran, diethyl ether, dioxane, etc.), amides (e.g., dimethylformamide, dimethylacetoamide, N-methylpyrolidone, etc.), and mixture thereof, etc.

The temperature for such reaction may be −10° C. to 150° C., preferably 0° C. to 80° C. Although reaction time depends on the compound, such reaction may be conducted for 10 minutes to 48 hours.

[Route 10]

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wherein R¹⁴and R¹⁵are each independently substituted or unsubstituted lower alkyl and the other variants are as defined above.

As shown, the compound of the invention represented by the general formula (Ij) may be prepared by reacting the compound (III), compound (IV), and compound (XIX) without solvent or in an appropriate solvent, in the presence or absence of an acid.

The compound (XIX) may be prepared by reacting the compound (XVII) and the compound (XVIII) without solvent or in an appropriate solvent, in the presence or absence of a base.

In this reaction, the compound (XVII) can be used in an amount of 1 or more equivalents, preferably 1 to 3 equivalents, in respect of compound (XVIII).

Base that may be used includes sodium hydride, sodium methoxide, potassium t-butoxide and the like.

Solvent that may be used includes alcohols (e.g., methanol, enthanol, etc.), aromatic hydrocarbons (e.g., toluene, benzene, xylene, etc.), saturated hydrocarbons (e.g., cyclohexane, hexanes, etc.), ethers (e.g., tetrahydrofuran, diethyl ether, dioxane, etc.) and mixture thereof, etc.

The temperature for such reaction may be −10° C. to 150° C., preferably 20° C. to 100° C. Reaction time depends on the compound, such reaction may be conducted for 10 minutes to 80 hours.

Optionally, desired compound (Ia) thus obtained may be purified according to conventional methods (e.g., column chromatography, recrystallization, etc.).

In this reaction, compound (III) and compound (IV) may be used in an amount of one equivalent or more, preferably 1 to 3 equivalents, in respect of compound (XIX).

Acid that may be used includes acetic acid, p-toluenesulfonic acid, hydrochloric acid and the like.

The temperature for such reaction may be −10° C. to 150° C., preferably 20° C. to 100° C. Reaction time depends on the compound, such reaction may be conducted for 10 minutes to 80 hours.

Optionally, desired compound (Ia) thus obtained may be purified according to conventional methods (e.g., column chromatography, recrystallization, etc.).

The compounds of the invention can form salts with pharmaceutically acceptable acids or bases, such as salts with an inorganic acid such as hydrochloric acid, sulfuric acid, nitric acid, phosphoric acid, hydrofluoric acid, hydrobromic acid, etc.; salts with an organic acid such as formic acid, acetic acid, oxalic acid, succinic acid, maleic acid, tartaric acid, lactic acid, citric acid, fumaric acid, etc.; salts with an organic base such as ammonium, trimethyl ammonium, triethyl ammonium, etc.; salts with an alkali metal such as sodium, potassium, etc.; salts with an alkali earth metal such as calcium, magnesium, etc.

Also, the compounds of the invention and pharmaceutically acceptable salts thereof as described above can be prepared in a form of solvate (preferably hydrate) thereof. Such solvate includes solvates with an organic solvent and/or water. Any number of solvent molecules can be coordinated to form such solvate.

The compound (I) of the invention is not limited to certain isomer, and thus, all possible isomers and racemates are encompassed by the invention. Also, the invention is intended to encompass tautomers as shown bellow.

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The compound of the invention may be isolated enantiomer having certain configuration or a mixture thereof. For example, the compound of the invention can be isolated enantiomer having a certain configuration at position 5 of the pyrrolidinone ring or a mixture of such enantiomers. One skilled in the art can readily isolate an enantiomer having such certain configuration using conventional techniques such as recrystallization, enzyme reaction, chromatography, etc.

The compound of the invention represented above by the general formula (I) has an antagonizing action on P2X₃and/or P2X₂/₃receptor, and therefore, is useful as a therapeutic agent for diseases associated with a P2X₃and/or P2X₂/₃receptor. Since P2X₃and/or P2X₂/₃receptor is believed to associate with pain and diseases in urinary system (Nature 407, 26, 1011-1015 (2000), Nature, Vol. 407, No. 26, 1015-1017 (2000), Non-Patent Document 1, Non-Patent Document 2, etc.), the compound of the invention is useful in the treatment of, alleviation of symptoms or prevention of diseases, such as for example, pain associated with rheumatoid arthritis, pain associated with osteoarthritis, headache, migraine, orofacial pain, toothache, glossagra, pain associated with temporomandibular arthrosis, trigeminal neuralgia, shoulder pain, pain associated with hernia of intervertebral disk, pain associated with cervical spondylosis deformans, pain associated with spinal canal stenosis, pain associated with thoracic outlet syndrome, pain associated with traumatic brachial plexus injury syndrome, pain associated with shoulder-hand syndrome, pain associated with whiplash injury, chest pain, abdominal pain, colic pain, pain associated with cholelithiasis, pain associated with pancreatitis, pain associated with urinary calculosis, pain associated with irritable bowel syndrome, lumbar backache, sciatica, pain associated with bone fracture, pain associated with osteoporosis, joint pain, pain associated with gout, pain associated with cauda equina syndrome, pain associated with ankylosing spondylitis, sore muscle, pain associated with painful spasm, pain associated with myofascial pain syndrome, pain associated with fibromyalgia syndrome, pain associated with arteriosclerosis obliterans, pain associated with Buerger's disease, pain associated with Raynaud's phenomenon, pain associated with zoster, causalgic pain, pain associated with entrapment neuropathy, pain associated with carpal canal syndrome, pain associated with diabetes, pain associated with Guillain-Barre syndrome, pain associated with Hansen's disease, pain associated with drug therapy, pain associated with radiation therapy, pain associated with cord injury, pain associated with syringomyelia, pain associated with stroke, thalamic pain, pain associated with deafferentation, sympathetically-maintained pain, pain associated with ABC syndrome, pain associated with multiple sclerosis, pain associated with skin disease, cancer pain, postoperative pain, pain associated with injury, pain associated with gangrene, pain associated with somatoform disorder, pain associated with somatization disorder, pain associated with depression, pain associated with Parkinson's disease, knee joint pain, pain associated with arthritis, neuropathic pain such as menstrual pain, intermenstrual pain, labor pain, etc., inflammatory pain, nociceptive pain, psychogenic pain, and overactive bladder, incontinence, pollakiuria, urinary urgency, cystatrophia, prostatic hypertrophy, prostatitis, prostate pain, detrusor hyperreflesxia, dysuria, nervous pollakiuria, chronic prostatitis, chronic cystitis, etc.

The compound of the invention can be a drug with reduced side-effect such as effect on motor function because it has a high affinity for ATP receptor, especially P2X₃receptor, and also has high subtype selectivity and high selectivity for other receptors. Also, the compound of the invention is advantageous because of its high stability and high oral absorptivity, good bioavailability, low clearance, long half-life, prolonged duration of action, and/or low activity of hepatic enzyme inhibition, etc.

In another embodiment, the invention provides a pharmaceutical composition comprising an effective amount of the compound of the invention, in combination with a pharmaceutically acceptable carrier.

For use of the compound of the invention as a medicament, a pharmaceutical composition can be prepared according to conventional methods, using pharmaceutically acceptable carriers well known in the art, such as excipients, binders, disintegrants, lubricants, colourants, flavors, surfactants, etc.

For the pharmaceutical composition of the invention to be administered in the treatment of mammals including human, an appropriate unit dosage form may be selected depending on the purpose of the treatment and the route of administration. Specifically, such unit dosage form includes oral formulations such as tablet, coated tablet, powder, granule, capsule, liquid, pill, suspension, emulsion, etc., and parenteral formulations such as injectable solution, suppository, ointment, patch, aerosol, etc. Such unit dosage form can be formulated according to methods well known in the art.

The amount of the compound in a formulation can be varied depending on its dosage form, route for administration, dosing regimen, etc.

Means for administration of the pharmaceutical composition may be selected depending on dosage form, age, sex, body weight, severity of the disease, and other factors, etc., and route for administration can be selected from various routes such as oral, subcutaneous, transdermal, rectal, intranasal, buccal, etc.

Dose of the compound of the invention in a pharmaceutical composition of the invention can be determined depending on the choice of route for administration, age, sex, body weight, severity of the disease, the compound to be administered, and other factors, etc., and can be generally from 0.05 to 1000 mg/kg/day, preferably from 0.1 to 10 mg/kg/day, for oral administration to adults. For parenteral administration, dose can be varied widely depending on its route but generally from 0.005 to 100 mg/kg/day, preferably from 0.01 to 1 mg/kg/day. Such pharmaceutical composition of the invention may be administered once a day or in several times at a divided dosage in a day.

Preferred embodiments of the compound of the invention are represented by the formula (a) to (f):

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TABLE 1

R¹

R1A
COOEt

R1B
CF₃

R1C
SCF₃

R1D
isoxazol-3-yl

R1E
3-Me-isoxazol-5-yl

R1F
5-Me-isoxazol-3-yl

R1G
1,2,4-oxadiazol-3-yl

R1H
1,3,4-oxadiazol-2-yl

R1I
5-Me-1,2,4-oxadiazol-3-yl

R1J
3-Me-1,2,4-oxadiazol-5-yl

R1K
C(Me)═NOMe

R1L
CH═NOMe

R1M
2-oxazolinyl

R1N
2-thiazolinyl

R1O
2-thiazolyl

R1P
2- or 3-thienyl

R1Q
2- or 3-furyl

TABLE 2

R²

R2A
iPr

R2B
cPr

R2C
tBu

R2D
Ph

R2E
4-Cl or F—Ph

R2F
4-CF₃—Ph

R2G
4-Me₂N—Ph

R2H
2- or 3-thienyl

R2I
3-pyridyl

R2J
6-MeO-3-pyridyl

R2K
2- or 3- or 4-MeO—Ph

R2L
HOCH₂C(Me)₂

R2M
HOCOC(Me)₂

R2N
MeC(CH₂OH)₂

R2O
Me₂NCOC(Me)₂

R2P
MeNHCOC(Me)₂

R2Q
H₂NCOC(Me)₂

TABLE 3

Z

ZA
Me

ZB
Et

ZC
iPr

ZD
CHF₂

ZE
CF₃

ZF
HOCH₂CH₂

ZG
MeOCH₂CH₂

ZH
NCCH₂

ZI
MeSCH₂CH₂

ZJ
MeSOCH₂CH₂

ZK
Me₂NCH₂CH₂

ZL
AcNHCH2CH2

ZM
MsNHCH₂CH₂

ZN
EtOCOCH₂

ZO
HOCOCH₂

ZP
HOCOCH₂CH₂

ZQ
HOCOCH(Me)

ZR
HOCOC(Me)₂

ZS
Me₂NCOCH₂

ZT
MeHNCOCH₂

ZU
H₂NCOCH₂

TABLE 4

X

XA
CH

XB
N

TABLE 5

Y

YA
O

YB
S

wherein

Ac is acetyl, Ms is mesyl, Me is methyl, Et is ethyl, Pr is propyl, iPr is isopropyl, nBu is n-butyl, tBu is t-butyl, cPr is cyclopropyl, cBu is cyclobutyl, cPent is cyclopentyl, cHex is cyclohexyl, Ph is phenyl; and

the combination of R¹, R², Z, X and Y, i.e., (R1,R2,Z,X,Y), is any one of the following combinations:

(R1,R2,Z,X,Y)=(R1A,R2A,ZA,XA,YA), (R1B,R2A,ZA,XA,YA), (R1C,R2A,ZA,XA,YA), (R1D,R2A,ZA,XA,YA), (R1E,R2A,ZA,XA,YA), (R1F,R2A,ZA,XA,YA), (R1G,R2A,ZA,XA,YA), (R1H,R2A,ZA,XA,YA), (R1I,R2A,ZA,XA,YA), (R1J,R2A,ZA,XA,YA), (R1K,R2A,ZA,XA,YA), (R1L,R2A,ZA,XA,YA), (R1M,R2A,ZA,XA,YA), (R1N,R2A,ZA,XA,YA), (R1O,R2A,ZA,XA,YA), (R1P,R2A,ZA,XA,YA), (R1Q,R2A,ZA,XA,YA), (R1A,R2B,ZA,XA,YA), (R1B,R2B,ZA,XA,YA), (R1C,R2B,ZA,XA,YA), (R1D,R2B,ZA,XA,YA), (R1E,R2B,ZA,XA,YA), (R1F,R2B,ZA,XA,YA), (R1G,R2B,ZA,XA,YA), (R1H,R2B,ZA,XA,YA), (R1I,R2B,ZA,XA,YA), (R1J,R2B,ZA,XA,YA), (R1K,R2B,ZA,XA,YA), (R1L,R2B,ZA,XA,YA), (R1M,R2B,ZA,XA,YA), (R1N,R2B,ZA,XA,YA), (R1O,R2B,ZA,XA,YA), (R1P,R2B,ZA,XA,YA), (R1Q,R2B,ZA,XA,YA), (R1A,R22C,ZA,XA,YA), (R1B,R22C,ZA,XA,YA), (R1C,R22C,ZA,XA,YA), (R1D,R22C,ZA,XA,YA), (R1E,R22C,ZA,XA,YA), (R1F,R22C,ZA,XA,YA), (R1G,R22C,ZA,XA,YA), (R1H,R22C,ZA,XA,YA), (R1I,R22C,ZA,XA,YA), (R1J,R22C,ZA,XA,YA), (R1K,R22C,ZA,XA,YA), (R1L,R22C,ZA,XA,YA), (R1M,R2C,ZA,XA,YA), (R1N,R22C,ZA,XA,YA), (R1O,R22C,ZA,XA,YA), (R1P,R22C,ZA,XA,YA), (R1Q,R22C,ZA,XA,YA), (R1A,R2D,ZA,XA,YA), (R1B,R2D,ZA,XA,YA), (R1C,R2D,ZA,XA,YA), (R1D,R2D,ZA,XA,YA), (R1E,R2D,ZA,XA,YA), (R1F,R2D,ZA,XA,YA), (R1G,R2D,ZA,XA,YA), (R1H,R2D,ZA,XA,YA), (R1I,R2D,ZA,XA,YA), (R1J,R2D,ZA,XA,YA), (R1K,R2D,ZA,XA,YA), (R1L,R2D,ZA,XA,YA), (R1M,R2D,ZA,XA,YA), (R1N,R2D,ZA,XA,YA), (R1O,R2D,ZA,XA,YA), (R1P,R2D,ZA,XA,YA), (R1Q,R2D,ZA,XA,YA), (R1A,R2E,ZA,XA,YA), (R1B,R2E,ZA,XA,YA), (R1C,R2E,ZA,XA,YA), (R1D,R2E,ZA,XA,YA), (R1E,R2E,ZA,XA,YA), (R1F,R2E,ZA,XA,YA), (R1G,R2E,ZA,XA,YA), (R1H,R2E,ZA,XA,YA), (R1I,R2E,ZA,XA,YA), (R1J,R2E,ZA,XA,YA), (R1K,R2E,ZA,XA,YA), (R1L,R2E,ZA,XA,YA), (R1M,R2E,ZA,XA,YA), (R1N,R2E,ZA,XA,YA), (R1O,R2E,ZA,XA,YA), (R1P,R2E,ZA,XA,YA), (R1Q,R2E,ZA,XA,YA), (R1A,R2F,ZA,XA,YA), (R1B,R2F,ZA,XA,YA), (R1C,R2F,ZA,XA,YA), (R1D,R2F,ZA,XA,YA), (R1E,R2F,ZA,XA,YA), (R1,R2F,ZA,XA,YA), (R1G,R2F,ZA,XA,YA), (R1H,R2F,ZA,XA,YA), (R1I,R2F,ZA,XA,YA), (R1J,R2F,ZA,XA,YA), (R1K,R2F,ZA,XA,YA), (R1L,R2F,ZA,XA,YA), (R1M,R2F,ZA,XA,YA), (R1N,R2F,ZA,XA,YA), (R1O,R2F,ZA,XA,YA), (R1P,R2F,ZA,XA,YA), (R1Q,R2F,ZA,XA,YA), (R1A,R2G,ZA,XA,YA), (R1B,R2G,ZA,XA,YA), (R1C,R2G,ZA,XA,YA), (R1D,R2G,ZA,XA,YA), (R1E,R2G,ZA,XA,YA), (R1F,R2G,ZA,XA,YA), (R1G,R2G,ZA,XA,YA), (R1H,R2G,ZA,XA,YA), (R1I,R2G,ZA,XA,YA), (R1J,R2G,ZA,XA,YA), (R1K,R2G,ZA,XA,YA), (R1L,R2G,ZA,XA,YA), (R1M,R2G,ZA,XA,YA), (R1N,R2G,ZA,XA,YA), (R1O,R2G,ZA,XA,YA), (R1P,R2G,ZA,XA,YA), (R1Q,R2G,ZA,XA,YA), (R1A,R2H,ZA,XA,YA), (R1B,R2H,ZA,XA,YA), (R1C,R2H,ZA,XA,YA), (R1D,R2H,ZA,XA,YA), (R1E,R2H,ZA,XA,YA), (R1F,R2H,ZA,XA,YA), (R1G,R2H,ZA,XA,YA), (R1H,R2H,ZA,XA,YA), (R1I,R2H,ZA,XA,YA), (R1J,R2H,ZA,XA,YA), (R1K,R2H,ZA,XA,YA), (R1L,R2H,ZA,XA,YA), (R1M,R2H,ZA,XA,YA), (R1N,R2H,ZA,XA,YA), (R1O,R2H,ZA,XA,YA), (R1P,R2H,ZA,XA,YA), (R1Q,R2H,ZA,XA,YA), (R1A,R2I,ZA,XA,YA), (R1B,R2I,ZA,XA,YA), (R1C,R2I,ZA,XA,YA), (R1D,R2I,ZA,XA,YA), (R1E,R2I,ZA,XA,YA), (R1F,R2I,ZA,XA,YA), (R1G,R2I,ZA,XA,YA), (R1H,R2I,ZA,XA,YA), (R1I,R2I,ZA,XA,YA), (R1J,R2I,ZA,XA,YA), (R1K,R2I,ZA,XA,YA), (R1L,R2I,ZA,XA,YA), (R1M,R2I,ZA,XA,YA), (R1N,R2I,ZA,XA,YA), (R1O,R2I,ZA,XA,YA), (R1P,R2I,ZA,XA,YA), (R1Q,R2I,ZA,XA,YA), (R1A,R2J,ZA,XA,YA), (R1B,R2J,ZA,XA,YA), (R1C,R2J,ZA,XA,YA), (R1D,R2J,ZA,XA,YA), (R1E,R2J,ZA,XA,YA), (R1F,R2J,ZA,XA,YA), (R1G,R2J,ZA,XA,YA), (R1H,R2J,ZA,XA,YA), (R1I,R2J,ZA,XA,YA), (R1J,R2J,ZA,XA,YA), (R1K,R2J,ZA,XA,YA), (R1L,R2J,ZA,XA,YA), (R1M,R2J,ZA,XA,YA), (R1N,R2J,ZA,XA,YA), (R1O,R2J,ZA,XA,YA), (R1P,R2J,ZA,XA,YA), (R1Q,R2J,ZA,XA,YA), (R1A,R2K,ZA,XA,YA), (R1B,R2K,ZA,XA,YA), (R1C,R2K,ZA,XA,YA), (R1D,R2K,ZA,XA,YA), (R1E,R2K,ZA,XA,YA), (R1F,R2K,ZA,XA,YA), (R1G,R2K,ZA,XA,YA), (R1H,R2K,ZA,XA,YA), (R1I,R2K,ZA,XA,YA), (R1J,R2K,ZA,XA,YA), (R1K,R2K,ZA,XA,YA), (R1L,R2K,ZA,XA,YA), (R1M,R2K,ZA,XA,YA), (R1N,R2K,ZA,XA,YA), (R1O,R2K,ZA,XA,YA), (R1P,R2K,ZA,XA,YA), (R1Q,R2K,ZA,XA,YA), (R1A,R2L, ZA,XA,YA), (R1B,R2L,ZA,XA,YA), (R1C,R2L,ZA,XA,YA), (R1D,R2L,ZA,XA,YA), (R1E,R2L,ZA,XA,YA), (R1F,R2L,ZA,XA,YA), (R1G,R2L,ZA,XA,YA), (R1H,R2L,ZA,XA,YA), (R1I,R2L,ZA,XA,YA), (R1J,R2L,ZA,XA,YA), (R1K,R2L,ZA,XA,YA), (R1L,R2L,ZA,XA,YA), (R1M,R2L,ZA,XA,YA), (R1N,R2L,ZA,XA,YA), (R1O,R2L,ZA,XA,YA), (R1P,R2L,ZA,XA,YA), (R1Q,R2L,ZA,XA,YA), (R1A,R2M,ZA,XA,YA), (R1B,R2M,ZA,XA,YA), (R1C,R2M,ZA,XA,YA), (R1D,R2M,ZA,XA,YA), (R1E,R2M,ZA,XA,YA), (R1F,R2M,ZA,XA,YA), (R1G,R2M,ZA,XA,YA), (R1H,R2M,ZA,XA,YA), (R1I,R2M,ZA,XA,YA), (R1J,R2M,ZA,XA,YA), (R1K,R2M,ZA,XA,YA), (R1L,R2M,ZA,XA,YA), (R1M,R2M,ZA,XA,YA), (R1N,R2M,ZA,XA,YA), (R1O,R2M,ZA,XA,YA), (R1P,R2M,ZA,XA,YA), (R1Q,R2M,ZA,XA,YA), (R1A,R2N,ZA,XA,YA), (R1B,R2N,ZA,XA,YA), (R1C,R2N,ZA,XA,YA), (R1D,R2N,ZA,XA,YA), (R1E,R2N,ZA,XA,YA), (R1F,R2N,ZA,XA,YA), (R1G,R2N,ZA,XA,YA), (R1H,R2N,ZA,XA,YA), (R1I,R2N,ZA,XA,YA), (R1J,R2N,ZA,XA,YA), (R1K,R2N,ZA,XA,YA), (R1L,R2N,ZA,XA,YA), (R1M,R2N,ZA,XA,YA), (R1N,R2N,ZA,XA,YA), (R1O,R2N,ZA,XA,YA), (R1P,R2N,ZA,XA,YA), (R1Q,R2N,ZA,XA,YA), (R1A,R2O,ZA,XA,YA), (R1B,R2O,ZA,XA,YA), (R1C,R2O,ZA,XA,YA), (R1D,R2O,ZA,XA,YA), (R1E,R2O,ZA,XA,YA), (R1F,R2O,ZA,XA,YA), (R1G,R2O,ZA,XA,YA), (R1H,R2O,ZA,XA,YA), (R1I,R2O,ZA,XA,YA), (R1J,R2O,ZA,XA,YA), (R1K,R2O,ZA,XA,YA), (R1L,R2O,ZA,XA,YA), (R1M,R2O,ZA,XA,YA), (R1N,R2O,ZA,XA,YA), (R1O,R2O,ZA,XA,YA), (R1P,R2O,ZA,XA,YA), (R1Q,R2O,ZA,XA,YA), (R1A,R2P,ZA,XA,YA), (R1B,R2P,ZA,XA,YA), (R1C,R2P,ZA,XA,YA), (R1D,R2P,ZA,XA,YA), (R1E,R2P,ZA,XA,YA), (R1F,R2P,ZA,XA,YA), (R1G,R2P,ZA,XA,YA), (R1H,R2P,ZA,XA,YA), (R1I,R2P,ZA,XA,YA), (R1J,R2P,ZA,XA,YA), (R1K,R2P,ZA,XA,YA), (R1L,R2P,ZA,XA,YA), (R1M,R2P,ZA,XA,YA), (R1N,R2P,ZA,XA,YA), (R1O,R2P,ZA,XA,YA), (R1P,R2P,ZA,XA,YA), (R1Q,R2P,ZA,XA,YA), (R1A,R2Q,ZA,XA,YA), (R1B,R2Q,ZA,XA,YA), (R1C,R2Q,ZA,XA,YA), (R1D,R2Q,ZA,XA,YA), (R1E,R2Q,ZA,XA,YA), (R1F,R2Q,ZA,XA,YA), (R1G,R2Q,ZA,XA,YA), (R1H,R2Q,ZA,XA,YA), (R1I,R2Q,ZA,XA,YA), (R1J,R2Q,ZA,XA,YA), (R1K,R2Q,ZA,XA,YA), (R1L,R2Q,ZA,XA,YA), (R1M,R2Q,ZA,XA,YA), (R1N,R2Q,ZA,XA,YA), (R1O,R2Q,ZA,XA,YA), (R1P,R2Q,ZA,XA,YA), (R1Q,R2Q,ZA,XA,YA), (R1A,R2A,ZB,XA,YA), (R1B,R2A,ZB,XA,YA), (R1C,R2A,ZB,XA,YA), (R1D,R2A,ZB,XA,YA), (R1E,R2A,ZB,XA,YA), (R1F,R2A,ZB,XA,YA), (R1G,R2A,ZB,XA,YA), (R1H,R2A,ZB,XA,YA), (R1I,R2A,ZB,XA,YA), (R1J,R2A,ZB,XA,YA), (R1K,R2A,ZB,XA,YA), (R1L,R2A,ZB,XA,YA), (R1M,R2A,ZB,XA,YA), (R1N,R2A,ZB,XA,YA), (R1O,R2A,ZB,XA,YA), (R1P,R2A,ZB,XA,YA), (R1Q,R2A,ZB,XA,YA), (R1A,R2B,ZB,XA,YA), (R1B,R2B,ZB,XA,YA), (R1C,R2B,ZB,XA,YA), (R1D,R2B,ZB,XA,YA), (R1E,R2B,ZB,XA,YA), (R1F,R2B,ZB,XA,YA), (R1G,R2B,ZB,XA,YA), (R1H,R2B,ZB,XA,YA), (R1I,R2B,ZB,XA,YA), (R1J,R2B,ZB,XA,YA), (R1K,R2B,ZB,XA,YA), (R1L,R2B,ZB,XA,YA), (R1M,R2B,ZB,XA,YA), (R1N,R2B,ZB,XA,YA), (R1O,R2B,ZB,XA,YA), (R1P,R2B,ZB,XA,YA), (R1Q,R2B,ZB,XA,YA), (R1A,R22C,ZB,XA,YA), (R1B,R22C,ZB,XA,YA), (R1C,R22C,ZB,XA,YA), (R1D,R22C,ZB,XA,YA), (R1E,R22C,ZB,XA,YA), (R1F,R22C,ZB,XA,YA), (R1G,R22C,ZB,XA,YA), (R1H,R22C,ZB,XA,YA), (R1I,R22C,ZB,XA,YA), (R1J,R22C,ZB,XA,YA), (R1K,R22C,ZB,XA,YA), (R1L,R22C,ZB,XA,YA), (R1M,R22C,ZB,XA,YA), (R1N,R22C,ZB,XA,YA), (R1O,R22C,ZB,XA,YA), (R1P,R22C,ZB,XA,YA), (R1Q,R22C,ZB,XA,YA), (R1A,R2D,ZB,XA,YA), (R1B,R2D,ZB,XA,YA), (R1C,R2D,ZB,XA,YA), (R1D,R2D,ZB,XA,YA), (R1E,R2D,ZB,XA,YA), (R1F,R2D,ZB,XA,YA), (R1G,R2D,ZB,XA,YA), (R1H,R2D,ZB,XA,YA), (R1I,R2D,ZB,XA,YA), (R1J,R2D,ZB,XA,YA), (R1K,R2D,ZB,XA,YA), (R1L,R2D,ZB,XA,YA), (R1M,R2D,ZB,XA,YA), (R1N,R2D,ZB,XA,YA), (R1O,R2D,ZB,XA,YA), (R1P,R2D,ZB,XA,YA), (R1Q,R2D,ZB,XA,YA), (R1A,R2E,ZB,XA,YA), (R1B,R2E,ZB,XA,YA), (R1C,R2E,ZB,XA,YA), (R1D,R2E,ZB,XA,YA), (R1E,R2E,ZB,XA,YA), (R1F,R2E,ZB,XA,YA), (R1G,R2E,ZB,XA,YA), (R1H,R2E,ZB,XA,YA), (R1I,R2E,ZB,XA,YA), (R1J,R2E,ZB,XA,YA), (R1K,R2E,ZB,XA,YA), (R1L,R2E,ZB,XA,YA), (R1M,R2E,ZB,XA,YA), (R1N,R2E,ZB,XA,YA), (R1O,R2E,ZB,XA,YA), (R1P,R2E,ZB,XA,YA), (R1Q,R2E,ZB,XA,YA), (R1A,R2F,ZB,XA,YA), (R1B,R2F,ZB,XA,YA), (R1C,R2F,ZB,XA,YA), (R1D,R2F,ZB,XA,YA), (R1E,R2F,ZB,XA,YA), (R1F,R2F,ZB,XA,YA), (R1G,R2F,ZB,XA,YA), (R1H,R2F,ZB,XA,YA), (R1I,R2F,ZB,XA,YA), (R1J,R2F,ZB,XA,YA), (R1K,R2F,ZB,XA,YA), (R1L,R2F,ZB,XA,YA), (R1M,R2F,ZB,XA,YA), (R1N,R2F,ZB,XA,YA), (R1O,R2F,ZB,XA,YA), (R1P,R2F,ZB,XA,YA), (R1Q,R2F,ZB,XA,YA), (R1A,R2G,ZB,XA,YA), (R1B,R2G,ZB,XA,YA), (R1C,R2G,ZB,XA,YA), (R1D,R2G,ZB,XA,YA), (R1E,R2G,ZB,XA,YA), 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(R1E,R2O,ZT,XB,YB), (R1F,R2O,ZT,XB,YB), (R1G,R2O,ZT,XB,YB), (R1H,R2O,ZT,XB,YB), (R1I,R2O,ZT,XB,YB), (R1J,R2O,ZT,XB,YB), (R1K,R2O,ZT,XB,YB), (R1L,R2O,ZT,XB,YB), (R1M,R2O,ZT,XB,YB), (R1N,R2O,ZT,XB,YB), (R1O,R2O,ZT,XB,YB), (R1P,R2O,ZT,XB,YB), (R1Q,R2O,ZT,XB,YB), (R1A,R2P,ZT,XB,YB), (R1B,R2P,ZT,XB,YB), (R1C,R2P,ZT,XB,YB), (R1D,R2P,ZT,XB,YB), (R1E,R2P,ZT,XB,YB), (R1F,R2P,ZT,XB,YB), (R1G,R2P,ZT,XB,YB), (R1H,R2P,ZT,XB,YB), (R1I,R2P,ZT,XB,YB), (R1J,R2P,ZT,XB,YB), (R1K,R2P,ZT,XB,YB), (R1L,R2P,ZT,XB,YB), (R1M,R2P,ZT,XB,YB), (R1N,R2P,ZT,XB,YB), (R1O,R2P,ZT,XB,YB), (R1P,R2P,ZT,XB,YB), (R1Q,R2P,ZT,XB,YB), (R1A,R2Q,ZT,XB,YB), (R1B,R2Q,ZT,XB,YB), (R1C,R2Q,ZT,XB,YB), (R1D,R2Q,ZT,XB,YB), (R1E,R2Q,ZT,XB,YB), (R1F,R2Q,ZT,XB,YB), (R1G,R2Q,ZT,XB,YB), (R1H,R2Q,ZT,XB,YB), (R1I,R2Q,ZT,XB,YB), (R1J,R2Q,ZT,XB,YB), (R1K,R2Q,ZT,XB,YB), (R1L,R2Q,ZT,XB,YB), (R1M,R2Q,ZT,XB,YB), (R1N,R2Q,ZT,XB,YB), (R1O,R2Q,ZT,XB,YB), (R1P,R2Q,ZT,XB,YB), (R1Q,R2Q,ZT,XB,YB), (R1A,R2A,ZU,XB,YB), (R1B,R2A,ZU,XB,YB), (R1C,R2A,ZU,XB,YB), (R1D,R2A,ZU,XB,YB), (R1E,R2A,ZU,XB,YB), (R1F,R2A,ZU,XB,YB), (R1G,R2A,ZU,XB,YB), (R1H,R2A,ZU,XB,YB), (R1I,R2A,ZU,XB,YB), (R1J,R2A,ZU,XB,YB), (R1K,R2A,ZU,XB,YB), (R1L,R2A,ZU,XB,YB), (R1M,R2A,ZU,XB,YB), (R1N,R2A,ZU,XB,YB), (R1O,R2A,ZU,XB,YB), (R1P,R2A,ZU,XB,YB), (R1Q,R2A,ZU,XB,YB), (R1A,R2B,ZU,XB,YB), (R1B,R2B,ZU,XB,YB), (R1C,R2B,ZU,XB,YB), (R1D,R2B,ZU,XB,YB), (R1E,R2B,ZU,XB,YB), (R1F,R2B,ZU,XB,YB), (R1G,R2B,ZU,XB,YB), (R1H,R2B,ZU,XB,YB), (R1I,R2B,ZU,XB,YB), (R1J,R2B,ZU,XB,YB), (R1K,R2B,ZU,XB,YB), (R1L,R2B,ZU,XB,YB), (R1M,R2B,ZU,XB,YB), (R1N,R2B,ZU,XB,YB), (R1O,R2B,ZU,XB,YB), (R1P,R2B,ZU,XB,YB), (R1Q,R2B,ZU,XB,YB), (R1A,R22C,ZU,XB,YB), (R1B,R22C,ZU,XB,YB), (R1C,R22C,ZU,XB,YB), (R1D,R22C,ZU,XB,YB), (R1E,R22C,ZU,XB,YB), (R1F,R22C,ZU,XB,YB), (R1G,R22C,ZU,XB,YB), (R1H,R22C,ZU,XB,YB), (R1I,R22C,ZU,XB,YB), (R1J,R22C,ZU,XB,YB), (R1K,R22C,ZU,XB,YB), (R1L,R22C,ZU,XB,YB), (R1M,R22C,ZU,XB,YB), (R1N,R22C,ZU,XB,YB), (R1O,R2C,ZU,XB,YB), (R1P,R22C,ZU,XB,YB), (R1Q,R22C,ZU,XB,YB), (R1A,R2D,ZU,XB,YB), (R1B,R2D,ZU,XB,YB), (R1C,R2D,ZU,XB,YB), (R1D,R2D,ZU,XB,YB), (R1E,R2D,ZU,XB,YB), (R1F,R2D,ZU,XB,YB), (R1G,R2D,ZU,XB,YB), (R1H,R2D,ZU,XB,YB), (R1I,R2D,ZU,XB,YB), (R1J,R2D,ZU,XB,YB), (R1K,R2D,ZU,XB,YB), (R1L,R2D,ZU,XB,YB), (R1M,R2D,ZU,XB,YB), (R1N,R2D,ZU,XB,YB), (R1O,R2D,ZU,XB,YB), (R1P,R2D,ZU,XB,YB), (R1Q,R2D,ZU,XB,YB), (R1A,R2E,ZU,XB,YB), (R1B,R2E,ZU,XB,YB), (R1C,R2E,ZU,XB,YB), (R1D,R2E,ZU,XB,YB), (R1E,R2E,ZU,XB,YB), (R1F,R2E,ZU,XB,YB), (R1G,R2E,ZU,XB,YB), (R1H,R2E,ZU,XB,YB), (R1I,R2E,ZU,XB,YB), (R1J,R2E,ZU,XB,YB), (R1K,R2E,ZU,XB,YB), (R1L,R2E,ZU,XB,YB), (R1M,R2E,ZU,XB,YB), (R1N,R2E,ZU,XB,YB), (R1O,R2E,ZU,XB,YB), (R1P,R2E,ZU,XB,YB), (R1Q,R2E,ZU,XB,YB), (R1A,R2F,ZU,XB,YB), (R1B,R2F,ZU,XB,YB), (R1C,R2F,ZU,XB,YB), (R1D,R2F,ZU,XB,YB), (R1E,R2F,ZU,XB,YB), (R1F,R2F,ZU,XB,YB), (R1G,R2F,ZU,XB,YB), (R1H,R2F,ZU,XB,YB), (R1I,R2F,ZU,XB,YB), (R1J,R2F,ZU,XB,YB), (R1K,R2F,ZU,XB,YB), (R1L,R2F,ZU,XB,YB), (R1M,R2F,ZU,XB,YB), (R1N,R2F,ZU,XB,YB), (R1O,R2F,ZU,XB,YB), (R1P,R2F,ZU,XB,YB), (R1Q,R2F,ZU,XB,YB), (R1A,R2G,ZU,XB,YB), (R1B,R2G,ZU,XB,YB), (R1C,R2G,ZU,XB,YB), (R1D,R2G,ZU,XB,YB), (R1E,R2G,ZU,XB,YB), (R1F,R2G,ZU,XB,YB), (R1G,R2G,ZU,XB,YB), (R1H,R2G,ZU,XB,YB), (R1I,R2G,ZU,XB,YB), (R1J,R2G,ZU,XB,YB), (R1K,R2G,ZU,XB,YB), (R1L,R2G,ZU,XB,YB), (R1M,R2G,ZU,XB,YB), (R1N,R2G,ZU,XB,YB), (R1O,R2G,ZU,XB,YB), (R1P,R2G,ZU,XB,YB), (R1Q,R2G,ZU,XB,YB), (R1A,R2H,ZU,XB,YB), (R1B,R2H,ZU,XB,YB), (R1C,R2H,ZU,XB,YB), (R1D,R2H,ZU,XB,YB), (R1E,R2H,ZU,XB,YB), (R1F,R2H,ZU,XB,YB), (R1G,R2H,ZU,XB,YB), (R1H,R2H,ZU,XB,YB), (R1I,R2H,ZU,XB,YB), (R1J,R2H,ZU,XB,YB), (R1K,R2H,ZU,XB,YB), (R1L,R2H,ZU,XB,YB), (R1M,R2H,ZU,XB,YB), (R1N,R2H,ZU,XB,YB), (R1O,R2H,ZU,XB,YB), (R1P,R2H,ZU,XB,YB), (R1Q,R2H,ZU,XB,YB), (R1A,R2I,ZU,XB,YB), (R1B,R2I,ZU,XB,YB), (R1C,R2I,ZU,XB,YB), (R1D,R2I,ZU,XB,YB), (R1E,R2I,ZU,XB,YB), (R1F,R2I,ZU,XB,YB), (R1G,R2I,ZU,XB,YB), (R1H,R2I,ZU,XB,YB), (R1I,R2I,ZU,XB,YB), (R1J,R2I,ZU,XB,YB), (R1K,R2I,ZU,XB,YB), (R1L,R2I,ZU,XB,YB), (R1M,R2I,ZU,XB,YB), (R1N,R2I,ZU,XB,YB), (R1O,R2I,ZU,XB,YB), (R1P,R2I,ZU,XB,YB), (R1Q,R2I,ZU,XB,YB), (R1A,R2J,ZU,XB,YB), (R1B,R2J,ZU,XB,YB), (R1C,R2J,ZU,XB,YB), (R1D,R2J,ZU,XB,YB), (R1E,R2J,ZU,XB,YB), (R1F,R2J,ZU,XB,YB), (R1G,R2J,ZU,XB,YB), (R1H,R2J,ZU,XB,YB), (R1I,R2J,ZU,XB,YB), (R1J,R2J,ZU,XB,YB), (R1K,R2J,ZU,XB,YB), (R1L,R2J,ZU,XB,YB), (R1M,R2J,ZU,XB,YB), (R1N,R2J,ZU,XB,YB), (R1O,R2J,ZU,XB,YB), (R1P,R2J,ZU,XB,YB), (R1Q,R2J,ZU,XB,YB), (R1A,R2K,ZU,XB,YB), (R1B,R2K,ZU,XB,YB), (R1C,R2K,ZU,XB,YB), (R1D,R2K,ZU,XB,YB), (R1E,R2K,ZU,XB,YB), (R1F,R2K,ZU,XB,YB), (R1G,R2K,ZU,XB,YB), (R1H,R2K,ZU,XB,YB), (R1I,R2K,ZU,XB,YB), (R1J,R2K,ZU,XB,YB), (R1K,R2K,ZU,XB,YB), (R1L,R2K,ZU,XB,YB), (R1M,R2K,ZU,XB,YB), (R1N,R2K,ZU,XB,YB), (R1O,R2K,ZU,XB,YB), (R1P,R2K,ZU,XB,YB), (R1Q,R2K,ZU,XB,YB), (R1A,R2L,ZU,XB,YB), (R1B,R2L,ZU,XB,YB), (R1C,R2L,ZU,XB,YB), (R1D,R2L,ZU,XB,YB), (R1E,R2L,ZU,XB,YB), (R1F,R2L,ZU,XB,YB), (R1G,R2L,ZU,XB,YB), (R1H,R2L,ZU,XB,YB), (R1I,R2L,ZU,XB,YB), (R1J,R2L,ZU,XB,YB), (R1K,R2L,ZU,XB,YB), (R1L,R2L,ZU,XB,YB), (R1M,R2L,ZU,XB,YB), (R1N,R2L,ZU,XB,YB), (R1O,R2L,ZU,XB,YB), (R1P,R2L,ZU,XB,YB), (R1Q,R2L,ZU,XB,YB), (R1A,R2M,ZU,XB,YB), (R1B,R2M,ZU,XB,YB), (R1C,R2M,ZU,XB,YB), (R1D,R2M,ZU,XB,YB), (R1E,R2M,ZU,XB,YB), (R1F,R2M,ZU,XB,YB), (R1G,R2M,ZU,XB,YB), (R1H,R2M,ZU,XB,YB), (R1I,R2M,ZU,XB,YB), (R1J,R2M,ZU,XB,YB), (R1K,R2M,ZU,XB,YB), (R1L,R2M,ZU,XB,YB), (R1M,R2M,ZU,XB,YB), (R1N,R2M,ZU,XB,YB), (R1O,R2M,ZU,XB,YB), (R1P,R2M,ZU,XB,YB), (R1Q,R2M,ZU,XB,YB), (R1A,R2N,ZU,XB,YB), (R1B,R2N,ZU,XB,YB), (R1C,R2N,ZU,XB,YB), (R1D,R2N,ZU,XB,YB), (R1E,R2N,ZU,XB,YB), (R1F,R2N,ZU,XB,YB), (R1G,R2N,ZU,XB,YB), (R1H,R2N,ZU,XB,YB), (R1I,R2N,ZU,XB,YB), (R1J,R2N,ZU,XB,YB), (R1K,R2N,ZU,XB,YB), (R1L,R2N,ZU,XB,YB), (R1M,R2N,ZU,XB,YB), (R1N,R2N,ZU,XB,YB), (R1O,R2N,ZU,XB,YB), (R1P,R2N,ZU,XB,YB), (R1Q,R2N,ZU,XB,YB), (R1A,R2O,ZU,XB,YB), (R1B,R2O,ZU,XB,YB), (R1C,R2O,ZU,XB,YB), (R1D,R2O,ZU,XB,YB), (R1E,R2O,ZU,XB,YB), (R1F,R2O,ZU,XB,YB), (R1G,R2O,ZU,XB,YB), (R1H,R2O,ZU,XB,YB), (R1I,R2O,ZU,XB,YB), (R1J,R2O,ZU,XB,YB), (R1K,R2O,ZU,XB,YB), (R1L,R2O,ZU,XB,YB), (R1M,R2O,ZU,XB,YB), (R1N,R2O,ZU,XB,YB), (R1O,R2O,ZU,XB,YB), (R1P,R2O,ZU,XB,YB), (R1Q,R2O,ZU,XB,YB), (R1A,R2P,ZU,XB,YB), (R1B,R2P,ZU,XB,YB), (R1C,R2P,ZU,XB,YB), (R1D,R2P,ZU,XB,YB), (R1E,R2P,ZU,XB,YB), (R1F,R2P,ZU,XB,YB), (R1G,R2P,ZU,XB,YB), (R1H,R2P,ZU,XB,YB), (R1I,R2P,ZU,XB,YB), (R1J,R2P,ZU,XB,YB), (R1K,R2P,ZU,XB,YB), (R1L,R2P,ZU,XB,YB), (R1M,R2P,ZU,XB,YB), (R1N,R2P,ZU,XB,YB), (R1O,R2P,ZU,XB,YB), (R1P,R2P,ZU,XB,YB), (R1Q,R2P,ZU,XB,YB), (R1A,R2Q,ZU,XB,YB), (R1B,R2Q,ZU,XB,YB), (R1C,R2Q,ZU,XB,YB), (R1D,R2Q,ZU,XB,YB), (R1E,R2Q,ZU,XB,YB), (R1F,R2Q,ZU,XB,YB), (R1G,R2Q,ZU,XB,YB), (R1H,R2Q,ZU,XB,YB), (R1I,R2Q,ZU,XB,YB), (R1J,R2Q,ZU,XB,YB), (R1K,R2Q,ZU,XB,YB), (R1L,R2Q,ZU,XB,YB), (R1M,R2Q,ZU,XB,YB), (R1N,R2Q,ZU,XB,YB), (R1O,R2Q,ZU,XB,YB), (R1P,R2Q,ZU,XB,YB) and (R1Q,R2Q,ZU,XB,YB).

Other preferred embodiments of the compound of the invention are the compound having the following groups in the formula (a′) to (f′):

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TABLE 6

R^a1
R^a

R^a2
COOEt

R^a3
isoxazol-3-yl

R^a4
3-Me-isoxazol-5-yl

R^a5
5-Me-1,2,4-oxadiazol-3-yl

R^a6
3-Me-1,2,4-oxadiazol-5-yl

R^a7
2-thiazolynyl

R^a8
2-thiazolyl

R^a9
2- or 3-thienyl

R^a10
2- or 3-furyl

R^a11
5-Me-2- or 3-thienyl

R^a12
5-Me-2- or 3-furyl

R^a13
SMe

R^a14
1-pyrrolidinyl

R^a15
1-cyclopentyl

R^a16
1-cyclopentenyl

TABLE 7

R^b

R^b1
iPr

R^b2
iBu

R^b3
tBu

R^b4
HOCH₂C(Me)₂

R^b5
Me(CH₂OH)₂Me

R^b6
Me₂NCOC(Me)₂

R^b7
MeNHCOC(Me)₂

R^b8
H₂NCOC(Me)₂

TABLE 8

Z

Z1
(HOCH₂)₂CHCH₂O

Z2
c-PentylO

Z3
Et(Me)NCO

Z4
EtHNCO

Z5
EtO

Z6
EtOCH₂O

Z7
H₂NCO(CH₂)₂

Z8
H₂NCOCH₂O

Z9
HO(CH₂)₂O

Z10
HO(CH₂)₃O

Z11
i-BuO

Z12
i-PrHNCO(CH₂)₂

Z13
i-PrO

Z14
i-PrOCH₂

Z15
Me₂N(CH₂)₂O

Z16
Me₂NCO

Z17
Me₂NCO(CH₂)₂

Z18
Me₂NCOCH₂

Z19
Me₂NCOCH₂O

Z20
MeHNCO(CH₂)₂

Z21
MeNHCOCH₂O

Z22
MeO

Z23
MeO(CH₂)₂

Z24
MeO(CH₂)₂(Me)NCO

Z25
MeO(CH₂)₂O

Z26
MeO(CH₂)₂OCH₂

Z27
MeO(CH₂)₃O

Z28
MeOCH₂

Z29
MeOCH₂O

Z30
MeS

Z31
MeSO(CH₂)₂O

Z32
MeSO₂

Z33
Morpholino

Z34
NC

Z35
NC(CH₂)₂O

Z36
NCCH₂O

Z37

embedded image

Z38

Z39

TABLE 9

X

X1
CH

X2
N

The combination of Ra, Rb, X and Z (Ra,Rb,X,Z) is any one of the following combinations:

(Ra,Rb,X,Z)=(Ra1,Rb1,X1,Z1), (Ra1,Rb1,X1,Z2), (Ra1,Rb1,X1,Z3), (Ra1,Rb1,X1,Z4), (Ra1,Rb1,X1,Z5), (Ra1,Rb1,X1,Z6), (Ra1,Rb1,X1,Z7), (Ra1,Rb1,X1,Z8), (Ra1,Rb1,X1,Z9), (Ra1,Rb1,X1,Z10), (Ra1,Rb1,X1,Z11), (Ra1,Rb1,X1,Z12), (Ra1,Rb1,X1,Z13), (Ra1,Rb1,X1,Z14), (Ra1,Rb1,X1,Z15), (Ra1,Rb1,X1,Z16), (Ra1,Rb1,X1,Z17), (Ra1,Rb1,X1,Z18), (Ra1,Rb1,X1,Z19), (Ra1,Rb1,X1,Z20), (Ra1,Rb1,X1,Z21), (Ra1,Rb1,X1,Z22), (Ra1,Rb1,X1,Z23), (Ra1,Rb1,X1,Z24), (Ra1,Rb1,X1,Z25), (Ra1,Rb1,X1,Z26), (Ra1,Rb1,X1,Z27), (Ra1,Rb1,X1,Z28), (Ra1,Rb1,X1,Z29), (Ra1,Rb1,X1,Z30), (Ra1,Rb1,X1,Z31), (Ra1,Rb1,X1,Z32), (Ra1,Rb1,X1,Z33), (Ra1,Rb1,X1,Z34), (Ra1,Rb1,X1,Z35), (Ra1,Rb1,X1,Z36), (Ra1,Rb1,X1,Z37), (Ra1,Rb1,X1,Z38), (Ra1,Rb1,X1,Z39), (Ra1,Rb1,X2,Z1), (Ra1,Rb1,X2,Z2), (Ra1,Rb1,X2,Z3), (Ra1,Rb1,X2,Z4), (Ra1,Rb1,X2,Z5), (Ra1,Rb1,X2,Z6), (Ra1,Rb1,X2,Z7), (Ra1,Rb1,X2,Z8), (Ra1,Rb1,X2,Z9), (Ra1,Rb1,X2,Z10), (Ra1,Rb1,X2,Z11), (Ra1,Rb1,X2,Z12), (Ra1,Rb1,X2,Z13), (Ra1,Rb1,X2,Z14), (Ra1,Rb1,X2,Z15), (Ra1,Rb1,X2,Z16), (Ra1,Rb1,X2,Z17), (Ra1,Rb1,X2,Z18), (Ra1,Rb1,X2,Z19), (Ra1,Rb1,X2,Z20), (Ra1,Rb1,X2,Z21), (Ra1,Rb1,X2,Z22), (Ra1,Rb1,X2,Z23), (Ra1,Rb1,X2,Z24), (Ra1,Rb1,X2,Z25), (Ra1,Rb1,X2,Z26), (Ra1,Rb1,X2,Z27), (Ra1,Rb1,X2,Z28), (Ra1,Rb1,X2,Z29), (Ra1,Rb1,X2,Z30), (Ra1,Rb1,X2,Z31), (Ra1,Rb1,X2,Z32), (Ra1,Rb1,X2,Z33), (Ra1,Rb1,X2,Z34), (Ra1,Rb1,X2,Z35), (Ra1,Rb1,X2,Z36), (Ra1,Rb1,X2,Z37), (Ra1,Rb1,X2,Z38), (Ra1,Rb1,X2,Z39), (Ra1,Rb2,X1,Z1), (Ra1,Rb2,X1,Z2), (Ra1,Rb2,X1,Z3), (Ra1,Rb2,X1,Z4), (Ra1,Rb2,X1,Z5), (Ra1,Rb2,X1,Z6), (Ra1,Rb2,X1,Z7), (Ra1,Rb2,X1,Z8), (Ra1,Rb2,X1,Z9), (Ra1,Rb2,X1,Z10), (Ra1,Rb2,X1,Z11), (Ra1,Rb2,X1,Z12), (Ra1,Rb2,X1,Z13), (Ra1,Rb2,X1,Z14), (Ra1,Rb2,X1,Z15), (Ra1,Rb2,X1,Z16), (Ra1,Rb2,X1,Z17), (Ra1,Rb2,X1,Z18), (Ra1,Rb2,X1,Z19), (Ra1,Rb2,X1,Z20), (Ra1,Rb2,X1,Z21), (Ra1,Rb2,X1,Z22), (Ra1,Rb2,X1,Z23), (Ra1,Rb2,X1,Z24), (Ra1,Rb2,X1,Z25), (Ra1,Rb2,X1,Z26), (Ra1,Rb2,X1,Z27), (Ra1,Rb2,X1,Z28), (Ra1,Rb2,X1,Z29), (Ra1,Rb2,X1,Z30), (Ra1,Rb2,X1,Z31), (Ra1,Rb2,X1,Z32), (Ra1,Rb2,X1,Z33), (Ra1,Rb2,X1,Z34), (Ra1,Rb2,X1,Z35), (Ra1,Rb2,X1,Z36), (Ra1,Rb2,X1,Z37), (Ra1,Rb2,X1,Z38), (Ra1,Rb2,X1,Z39), (Ra1,Rb2,X2,Z1), (Ra1,Rb2,X2,Z2), (Ra1,Rb2,X2,Z3), (Ra1,Rb2,X2,Z4), (Ra1,Rb2,X2,Z5), (Ra1,Rb2,X2,Z6), (Ra1,Rb2,X2,Z7), (Ra1,Rb2,X2,Z8), (Ra1,Rb2,X2,Z9), (Ra1,Rb2,X2,Z10), (Ra1,Rb2,X2,Z11), (Ra1,Rb2,X2,Z12), (Ra1,Rb2,X2,Z13), (Ra1,Rb2,X2,Z14), (Ra1,Rb2,X2,Z15), (Ra1,Rb2,X2,Z16), (Ra1,Rb2,X2,Z17), (Ra1,Rb2,X2,Z18), (Ra1,Rb2,X2,Z19), (Ra1,Rb2,X2,Z20), (Ra1,Rb2,X2,Z21), (Ra1,Rb2,X2,Z22), (Ra1,Rb2,X2,Z23), (Ra1,Rb2,X2,Z24), (Ra1,Rb2,X2,Z25), (Ra1,Rb2,X2,Z26), (Ra1,Rb2,X2,Z27), (Ra1,Rb2,X2,Z28), (Ra1,Rb2,X2,Z29), (Ra1,Rb2,X2,Z30), (Ra1,Rb2,X2,Z31), (Ra1,Rb2,X2,Z32), (Ra1,Rb2,X2,Z33), (Ra1,Rb2,X2,Z34), (Ra1,Rb2,X2,Z35), (Ra1,Rb2,X2,Z36), (Ra1,Rb2,X2,Z37), (Ra1,Rb2,X2,Z38), (Ra1,Rb2,X2,Z39), (Ra1,Rb3,X1,Z1), (Ra1,Rb3,X1,Z2), (Ra1,Rb3,X1,Z3), (Ra1,Rb3,X1,Z4), (Ra1,Rb3,X1,Z5), (Ra1,Rb3,X1,Z6), (Ra1,Rb3,X1,Z7), (Ra1,Rb3,X1,Z8), (Ra1,Rb3,X1,Z9), (Ra1,Rb3,X1,Z10), (Ra1,Rb3,X1,Z11), (Ra1,Rb3,X1,Z12), (Ra1,Rb3,X1,Z13), (Ra1,Rb3,X1,Z14), (Ra1,Rb3,X1,Z15), (Ra1,Rb3,X1,Z16), (Ra1,Rb3,X1,Z17), (Ra1,Rb3,X1,Z18), (Ra1,Rb3,X1,Z19), (Ra1,Rb3,X1,Z20), (Ra1,Rb3,X1,Z21), (Ra1,Rb3,X1,Z22), (Ra1,Rb3,X1,Z23), (Ra1,Rb3,X1,Z24), (Ra1,Rb3,X1,Z25), (Ra1,Rb3,X1,Z26), (Ra1,Rb3,X1,Z27), (Ra1,Rb3,X1,Z28), (Ra1,Rb3,X1,Z29), (Ra1,Rb3,X1,Z30), (Ra1,Rb3,X1,Z31), (Ra1,Rb3,X1,Z32), (Ra1,Rb3,X1,Z33), (Ra1,Rb3,X1,Z34), (Ra1,Rb3,X1,Z35), (Ra1,Rb3,X1,Z36), (Ra1,Rb3,X1,Z37), (Ra1,Rb3,X1,Z38), (Ra1,Rb3,X1,Z39), (Ra1,Rb3,X2,Z1), (Ra1,Rb3,X2,Z2), (Ra1,Rb3,X2,Z3), (Ra1,Rb3,X2,Z4), (Ra1,Rb3,X2,Z5), (Ra1,Rb3,X2,Z6), (Ra1,Rb3,X2,Z7), (Ra1,Rb3,X2,Z8), (Ra1,Rb3,X2,Z9), (Ra1,Rb3,X2,Z10), (Ra1,Rb3,X2,Z11), (Ra1,Rb3,X2,Z12), (Ra1,Rb3,X2,Z13), (Ra1,Rb3,X2,Z14), (Ra1,Rb3,X2,Z15), (Ra1,Rb3,X2,Z16), (Ra1,Rb3,X2,Z17), (Ra1,Rb3,X2,Z18), (Ra1,Rb3,X2,Z19), (Ra1,Rb3,X2,Z20), (Ra1,Rb3,X2,Z21), (Ra1,Rb3,X2,Z22), (Ra1,Rb3,X2,Z23), (Ra1,Rb3,X2,Z24), (Ra1,Rb3,X2,Z25), (Ra1,Rb3,X2,Z26), (Ra1,Rb3,X2,Z27), (Ra1,Rb3,X2,Z28), (Ra1,Rb3,X2,Z29), (Ra1,Rb3,X2,Z30), (Ra1,Rb3,X2,Z31), (Ra1,Rb3,X2,Z32), (Ra1,Rb3,X2,Z33), (Ra1,Rb3,X2,Z34), (Ra1,Rb3,X2,Z35), (Ra1,Rb3,X2,Z36), (Ra1,Rb3,X2,Z37), (Ra1,Rb3,X2,Z38), (Ra1,Rb3,X2,Z39), (Ra1,Rb4,X1,Z1), (Ra1,Rb4,X1,Z2), (Ra1,Rb4,X1,Z3), (Ra1,Rb4,X1,Z4), (Ra1,Rb4,X1,Z5), (Ra1,Rb4,X1,Z6), (Ra1,Rb4,X1,Z7), (Ra1,Rb4,X1,Z8), (Ra1,Rb4,X1,Z9), (Ra1,Rb4,X1,Z10), (Ra1,Rb4,X1,Z11), (Ra1,Rb4,X1,Z12), (Ra1,Rb4,X1,Z13), (Ra1,Rb4,X1,Z14), (Ra1,Rb4,X1,Z15), (Ra1,Rb4,X1,Z16), (Ra1,Rb4,X1,Z17), (Ra1,Rb4,X1,Z18), (Ra1,Rb4,X1,Z19), (Ra1,Rb4,X1,Z20), (Ra1,Rb4,X1,Z21), (Ra1,Rb4,X1,Z22), (Ra1,Rb4,X1,Z23), (Ra1,Rb4,X1,Z24), (Ra1,Rb4,X1,Z25), (Ra1,Rb4,X1,Z26), (Ra1,Rb4,X1,Z27), (Ra1,Rb4,X1,Z28), (Ra1,Rb4,X1,Z29), (Ra1,Rb4,X1,Z30), (Ra1,Rb4,X1,Z31), (Ra1,Rb4,X1,Z32), (Ra1,Rb4,X1,Z33), (Ra1,Rb4,X1,Z34), (Ra1,Rb4,X1,Z35), (Ra1,Rb4,X1,Z36), (Ra1,Rb4,X1,Z37), (Ra1,Rb4,X1,Z38), (Ra1,Rb4,X1,Z39), (Ra1,Rb4,X2,Z1), (Ra1,Rb4,X2,Z2), (Ra1,Rb4,X2,Z3), (Ra1,Rb4,X2,Z4), (Ra1,Rb4,X2,Z5), (Ra1,Rb4,X2,Z6), (Ra1,Rb4,X2,Z7), (Ra1,Rb4,X2,Z8), (Ra1,Rb4,X2,Z9), (Ra1,Rb4,X2,Z10), (Ra1,Rb4,X2,Z11), (Ra1,Rb4,X2,Z12), (Ra1,Rb4,X2,Z13), (Ra1,Rb4,X2,Z14), (Ra1,Rb4,X2,Z15), (Ra1,Rb4,X2,Z16), (Ra1,Rb4,X2,Z17), (Ra1,Rb4,X2,Z18), (Ra1,Rb4,X2,Z19), (Ra1,Rb4,X2,Z20), (Ra1,Rb4,X2,Z21), (Ra1,Rb4,X2,Z22), (Ra1,Rb4,X2,Z23), (Ra1,Rb4,X2,Z24), (Ra1,Rb4,X2,Z25), (Ra1,Rb4,X2,Z26), (Ra1,Rb4,X2,Z27), (Ra1,Rb4,X2,Z28), (Ra1,Rb4,X2,Z29), (Ra1,Rb4,X2,Z30), (Ra1,Rb4,X2,Z31), (Ra1,Rb4,X2,Z32), (Ra1,Rb4,X2,Z33), (Ra1,Rb4,X2,Z34), (Ra1,Rb4,X2,Z35), (Ra1,Rb4,X2,Z36), (Ra1,Rb4,X2,Z37), (Ra1,Rb4,X2,Z38), (Ra1,Rb4,X2,Z39), (Ra1,Rb5,X1,Z1), (Ra1,Rb5,X1,Z2), (Ra1,Rb5,X1,Z3), (Ra1,Rb5,X1,Z4), (Ra1,Rb5,X1,Z5), (Ra1,Rb5,X1,Z6), (Ra1,Rb5,X1,Z7), (Ra1,Rb5,X1,Z8), (Ra1,Rb5,X1,Z9), (Ra1,Rb5,X1,Z10), (Ra1,Rb5,X1,Z11), (Ra1,Rb5,X1,Z12), (Ra1,Rb5,X1,Z13), (Ra1,Rb5,X1,Z14), (Ra1,Rb5,X1,Z15), (Ra1,Rb5,X1,Z16), (Ra1,Rb5,X1,Z17), (Ra1,Rb5,X1,Z18), (Ra1,Rb5,X1,Z19), (Ra1,Rb5,X1,Z20), (Ra1,Rb5,X1,Z21), (Ra1,Rb5,X1,Z22), (Ra1,Rb5,X1,Z23), (Ra1,Rb5,X1,Z24), (Ra1,Rb5,X1,Z25), (Ra1,Rb5,X1,Z26), (Ra1,Rb5,X1,Z27), (Ra1,Rb5,X1,Z28), (Ra1,Rb5,X1,Z29), (Ra1,Rb5,X1,Z30), (Ra1,Rb5,X1,Z31), (Ra1,Rb5,X1,Z32), (Ra1,Rb5,X1,Z33), (Ra1,Rb5,X1,Z34), (Ra1,Rb5,X1,Z35), (Ra1,Rb5,X1,Z36), (Ra1,Rb5,X1,Z37), (Ra1,Rb5,X1,Z38), (Ra1,Rb5,X1,Z39), (Ra1,Rb5,X2,Z1), (Ra1,Rb5,X2,Z2), (Ra1,Rb5,X2,Z3), (Ra1,Rb5,X2,Z4), (Ra1,Rb5,X2,Z5), (Ra1,Rb5,X2,Z6), (Ra1,Rb5,X2,Z7), (Ra1,Rb5,X2,Z8), (Ra1,Rb5,X2,Z9), (Ra1,Rb5,X2,Z10), (Ra1,Rb5,X2,Z11), (Ra1,Rb5,X2,Z12), (Ra1,Rb5,X2,Z13), (Ra1,Rb5,X2,Z14), (Ra1,Rb5,X2,Z15), (Ra1,Rb5,X2,Z16), (Ra1,Rb5,X2,Z17), (Ra1,Rb5,X2,Z18), (Ra1,Rb5,X2,Z19), (Ra1,Rb5,X2,Z20), (Ra1,Rb5,X2,Z21), (Ra1,Rb5,X2,Z22), (Ra1,Rb5,X2,Z23), (Ra1,Rb5,X2,Z24), (Ra1,Rb5,X2,Z25), (Ra1,Rb5,X2,Z26), (Ra1,Rb5,X2,Z27), (Ra1,Rb5,X2,Z28), (Ra1,Rb5,X2,Z29), (Ra1,Rb5,X2,Z30), (Ra1,Rb5,X2,Z31), (Ra1,Rb5,X2,Z32), (Ra1,Rb5,X2,Z33), (Ra1,Rb5,X2,Z34), (Ra1,Rb5,X2,Z35), (Ra1,Rb5,X2,Z36), (Ra1,Rb5,X2,Z37), (Ra1,Rb5,X2,Z38), (Ra1,Rb5,X2,Z39), (Ra1,Rb6,X1,Z1), (Ra1,Rb6,X1,Z2), (Ra1,Rb6,X1,Z3), (Ra1,Rb6,X1,Z4), (Ra1,Rb6,X1,Z5), (Ra1,Rb6,X1,Z6), (Ra1,Rb6,X1,Z7), (Ra1,Rb6,X1,Z8), (Ra1,Rb6,X1,Z9), (Ra1,Rb6,X1,Z10), (Ra1,Rb6,X1,Z11), (Ra1,Rb6,X1,Z12), (Ra1,Rb6,X1,Z13), (Ra1,Rb6,X1,Z14), (Ra1,Rb6,X1,Z15), (Ra1,Rb6,X1,Z16), (Ra1,Rb6,X1,Z17), (Ra1,Rb6,X1,Z18), (Ra1,Rb6,X1,Z19), (Ra1,Rb6,X1,Z20), (Ra1,Rb6,X1,Z21), (Ra1,Rb6,X1,Z22), (Ra1,Rb6,X1,Z23), (Ra1,Rb6,X1,Z24), (Ra1,Rb6,X1,Z25), (Ra1,Rb6,X1,Z26), (Ra1,Rb6,X1,Z27), (Ra1,Rb6,X1,Z28), (Ra1,Rb6,X1,Z29), (Ra1,Rb6,X1,Z30), (Ra1,Rb6,X1,Z31), (Ra1,Rb6,X1,Z32), (Ra1,Rb6,X1,Z33), (Ra1,Rb6,X1,Z34), (Ra1,Rb6,X1,Z35), (Ra1,Rb6,X1,Z36), (Ra1,Rb6,X1,Z37), (Ra1,Rb6,X1,Z38), (Ra1,Rb6,X1,Z39), (Ra1,Rb6,X2,Z1), (Ra1,Rb6,X2,Z2), (Ra1,Rb6,X2,Z3), (Ra1,Rb6,X2,Z4), (Ra1,Rb6,X2,Z5), (Ra1,Rb6,X2,Z6), (Ra1,Rb6,X2,Z7), (Ra1,Rb6,X2,Z8), (Ra1,Rb6,X2,Z9), (Ra1,Rb6,X2,Z10), (Ra1,Rb6,X2,Z11), (Ra1,Rb6,X2,Z12), (Ra1,Rb6,X2,Z13), (Ra1,Rb6,X2,Z14), (Ra1,Rb6,X2,Z15), (Ra1,Rb6,X2,Z16), (Ra1,Rb6,X2,Z17), (Ra1,Rb6,X2,Z18), (Ra1,Rb6,X2,Z19), (Ra1,Rb6,X2,Z20), (Ra1,Rb6,X2,Z21), (Ra1,Rb6,X2,Z22), (Ra1,Rb6,X2,Z23), (Ra1,Rb6,X2,Z24), (Ra1,Rb6,X2,Z25), (Ra1,Rb6,X2,Z26), (Ra1,Rb6,X2,Z27), (Ra1,Rb6,X2,Z28), (Ra1,Rb6,X2,Z29), (Ra1,Rb6,X2,Z30), (Ra1,Rb6,X2,Z31), (Ra1,Rb6,X2,Z32), (Ra1,Rb6,X2,Z33), (Ra1,Rb6,X2,Z34), (Ra1,Rb6,X2,Z35), (Ra1,Rb6,X2,Z36), (Ra1,Rb6,X2,Z37), (Ra1,Rb6,X2,Z38), (Ra1,Rb6,X2,Z39), (Ra1,Rb7,X1,Z1), (Ra1,Rb7,X1,Z2), (Ra1,Rb7,X1,Z3), (Ra1,Rb7,X1,Z4), (Ra1,Rb7,X1,Z5), (Ra1,Rb7,X1,Z6), (Ra1,Rb7,X1,Z7), (Ra1,Rb7,X1,Z8), (Ra1,Rb7,X1,Z9), (Ra1,Rb7,X1,Z10), (Ra1,Rb7,X1,Z11), (Ra1,Rb7,X1,Z12), (Ra1,Rb7,X1,Z13), (Ra1,Rb7,X1,Z14), (Ra1,Rb7,X1,Z15), (Ra1,Rb7,X1,Z16), (Ra1,Rb7,X1,Z17), (Ra1,Rb7,X1,Z18), (Ra1,Rb7,X1,Z19), (Ra1,Rb7,X1,Z20), (Ra1,Rb7,X1,Z21), (Ra1,Rb7,X1,Z22), (Ra1,Rb7,X1,Z23), (Ra1,Rb7,X1,Z24), (Ra1,Rb7,X1,Z25), (Ra1,Rb7,X1,Z26), (Ra1,Rb7,X1,Z27), (Ra1,Rb7,X1,Z28), (Ra1,Rb7,X1,Z29), (Ra1,Rb7,X1,Z30), (Ra1,Rb7,X1,Z31), (Ra1,Rb7,X1,Z32), (Ra1,Rb7,X1,Z33), (Ra1,Rb7,X1,Z34), (Ra1,Rb7,X1,Z35), (Ra1,Rb7,X1,Z36), (Ra1,Rb7,X1,Z37), (Ra1,Rb7,X1,Z38), (Ra1,Rb7,X1,Z39), (Ra1,Rb7,X2,Z1), (Ra1,Rb7,X2,Z2), (Ra1,Rb7,X2,Z3), (Ra1,Rb7,X2,Z4), (Ra1,Rb7,X2,Z5), (Ra1,Rb7,X2,Z6), (Ra1,Rb7,X2,Z7), (Ra1,Rb7,X2,Z8), (Ra1,Rb7,X2,Z9), (Ra1,Rb7,X2,Z10), (Ra1,Rb7,X2,Z11), (Ra1,Rb7,X2,Z12), (Ra1,Rb7,X2,Z13), (Ra1,Rb7,X2,Z14), (Ra1,Rb7,X2,Z15), (Ra1,Rb7,X2,Z16), (Ra1,Rb7,X2,Z17), (Ra1,Rb7,X2,Z18), (Ra1,Rb7,X2,Z19), (Ra1,Rb7,X2,Z20), (Ra1,Rb7,X2,Z21), (Ra1,Rb7,X2,Z22), (Ra1,Rb7,X2,Z23), (Ra1,Rb7,X2,Z24), (Ra1,Rb7,X2,Z25), (Ra1,Rb7,X2,Z26), (Ra1,Rb7,X2,Z27), (Ra1,Rb7,X2,Z28), (Ra1,Rb7,X2,Z29), (Ra1,Rb7,X2,Z30), (Ra1,Rb7,X2,Z31), (Ra1,Rb7,X2,Z32), (Ra1,Rb7,X2,Z33), (Ra1,Rb7,X2,Z34), (Ra1,Rb7,X2,Z35), (Ra1,Rb7,X2,Z36), (Ra1,Rb7,X2,Z37), (Ra1,Rb7,X2,Z38), (Ra1,Rb7,X2,Z39), (Ra1,Rb8,X1,Z1), (Ra1,Rb8,X1,Z2), (Ra1,Rb8,X1,Z3), (Ra1,Rb8,X1,Z4), (Ra1,Rb8,X1,Z5), (Ra1,Rb8,X1,Z6), (Ra1,Rb8,X1,Z7), (Ra1,Rb8,X1,Z8), (Ra1,Rb8,X1,Z9), (Ra1,Rb8,X1,Z10), (Ra1,Rb8,X1,Z11), (Ra1,Rb8,X1,Z12), (Ra1,Rb8,X1,Z13), (Ra1,Rb8,X1,Z14), (Ra1,Rb8,X1,Z15), (Ra1,Rb8,X1,Z16), (Ra1,Rb8,X1,Z17), (Ra1,Rb8,X1,Z18), (Ra1,Rb8,X1,Z19), (Ra1,Rb8,X1,Z20), (Ra1,Rb8,X1,Z21), (Ra1,Rb8,X1,Z22), (Ra1,Rb8,X1,Z23), (Ra1,Rb8,X1,Z24), (Ra1,Rb8,X1,Z25), (Ra1,Rb8,X1,Z26), (Ra1,Rb8,X1,Z27), (Ra1,Rb8,X1,Z28), (Ra1,Rb8,X1,Z29), (Ra1,Rb8,X1,Z30), (Ra1,Rb8,X1,Z31), (Ra1,Rb8,X1,Z32), (Ra1,Rb8,X1,Z33), (Ra1,Rb8,X1,Z34), (Ra1,Rb8,X1,Z35), (Ra1,Rb8,X1,Z36), (Ra1,Rb8,X1,Z37), (Ra1,Rb8,X1,Z38), (Ra1,Rb8,X1,Z39), (Ra1,Rb8,X2,Z1), (Ra1,Rb8,X2,Z2), (Ra1,Rb8,X2,Z3), (Ra1,Rb8,X2,Z4), (Ra1,Rb8,X2,Z5), (Ra1,Rb8,X2,Z6), (Ra1,Rb8,X2,Z7), (Ra1,Rb8,X2,Z8), (Ra1,Rb8,X2,Z9), (Ra1,Rb8,X2,Z10), (Ra1,Rb8,X2,Z11), (Ra1,Rb8,X2,Z12), (Ra1,Rb8,X2,Z13), (Ra1,Rb8,X2,Z14), (Ra1,Rb8,X2,Z15), (Ra1,Rb8,X2,Z16), (Ra1,Rb8,X2,Z17), (Ra1,Rb8,X2,Z18), (Ra1,Rb8,X2,Z19), (Ra1,Rb8,X2,Z20), (Ra1,Rb8,X2,Z21), (Ra1,Rb8,X2,Z22), (Ra1,Rb8,X2,Z23), (Ra1,Rb8,X2,Z24), (Ra1,Rb8,X2,Z25), (Ra1,Rb8,X2,Z26), (Ra1,Rb8,X2,Z27), (Ra1,Rb8,X2,Z28), (Ra1,Rb8,X2,Z29), (Ra1,Rb8,X2,Z30), (Ra1,Rb8,X2,Z31), (Ra1,Rb8,X2,Z32), (Ra1,Rb8,X2,Z33), (Ra1,Rb8,X2,Z34), (Ra1,Rb8,X2,Z35), (Ra1,Rb8,X2,Z36), (Ra1,Rb8,X2,Z37), (Ra1,Rb8,X2,Z38), (Ra1,Rb8,X2,Z39), (Ra2,Rb1,X1,Z1), (Ra2,Rb1,X1,Z2), (Ra2,Rb1,X1,Z3), (Ra2,Rb1,X1,Z4), (Ra2,Rb1,X1,Z5), (Ra2,Rb1,X1,Z6), (Ra2,Rb1,X1,Z7), (Ra2,Rb1,X1,Z8), (Ra2,Rb1,X1,Z9), (Ra2,Rb1,X1,Z10), (Ra2,Rb1,X1,Z11), (Ra2,Rb1,X1,Z12), (Ra2,Rb1,X1,Z13), (Ra2,Rb1,X1,Z14), (Ra2,Rb1,X1,Z15), (Ra2,Rb1,X1,Z16), (Ra2,Rb1,X1,Z17), (Ra2,Rb1,X1,Z18), (Ra2,Rb1,X1,Z19), (Ra2,Rb1,X1,Z20), (Ra2,Rb1,X1,Z21), (Ra2,Rb1,X1,Z22), (Ra2,Rb1,X1,Z23), (Ra2,Rb1,X1,Z24), (Ra2,Rb1,X1,Z25), (Ra2,Rb1,X1,Z26), (Ra2,Rb1,X1,Z27), (Ra2,Rb1,X1,Z28), (Ra2,Rb1,X1,Z29), (Ra2,Rb1,X1,Z30), (Ra2,Rb1,X1,Z31), (Ra2,Rb1,X1,Z32), (Ra2,Rb1,X1,Z33), (Ra2,Rb1,X1,Z34), (Ra2,Rb1,X1,Z35), (Ra2,Rb1,X1,Z36), (Ra2,Rb1,X1,Z37), (Ra2,Rb1,X1,Z38), (Ra2,Rb1,X1,Z39), (Ra2,Rb1,X2,Z1), (Ra2,Rb1,X2,Z2), (Ra2,Rb1,X2,Z3), (Ra2,Rb1,X2,Z4), (Ra2,Rb1,X2,Z5), (Ra2,Rb1,X2,Z6), (Ra2,Rb1,X2,Z7), (Ra2,Rb1,X2,Z8), (Ra2,Rb1,X2,Z9), (Ra2,Rb1,X2,Z10), (Ra2,Rb1,X2,Z11), (Ra2,Rb1,X2,Z12), (Ra2,Rb1,X2,Z13), (Ra2,Rb1,X2,Z14), (Ra2,Rb1,X2,Z15), (Ra2,Rb1,X2,Z16), (Ra2,Rb1,X2,Z17), (Ra2,Rb1,X2,Z18), (Ra2,Rb1,X2,Z19), (Ra2,Rb1,X2,Z20), (Ra2,Rb1,X2,Z21), (Ra2,Rb1,X2,Z22), (Ra2,Rb1,X2,Z23), (Ra2,Rb1,X2,Z24), (Ra2,Rb1,X2,Z25), (Ra2,Rb1,X2,Z26), (Ra2,Rb1,X2,Z27), (Ra2,Rb1,X2,Z28), (Ra2,Rb1,X2,Z29), (Ra2,Rb1,X2,Z30), (Ra2,Rb1,X2,Z31), (Ra2,Rb1,X2,Z32), (Ra2,Rb1,X2,Z33), (Ra2,Rb1,X2,Z34), (Ra2,Rb1,X2,Z35), (Ra2,Rb1,X2,Z36), (Ra2,Rb1,X2,Z37), (Ra2,Rb1,X2,Z38), (Ra2,Rb1,X2,Z39), (Ra2,Rb2,X1,Z1), (Ra2,Rb2,X1,Z2), (Ra2,Rb2,X1,Z3), (Ra2,Rb2,X1,Z4), (Ra2,Rb2,X1,Z5), (Ra2,Rb2,X1,Z6), (Ra2,Rb2,X1,Z7), (Ra2,Rb2,X1,Z8), (Ra2,Rb2,X1,Z9), (Ra2,Rb2,X1,Z10), (Ra2,Rb2,X1,Z11), (Ra2,Rb2,X1,Z12), (Ra2,Rb2,X1,Z13), (Ra2,Rb2,X1,Z14), (Ra2,Rb2,X1,Z15), (Ra2,Rb2,X1,Z16), (Ra2,Rb2,X1,Z17), (Ra2,Rb2,X1,Z18), (Ra2,Rb2,X1,Z19), (Ra2,Rb2,X1,Z20), (Ra2,Rb2,X1,Z21), (Ra2,Rb2,X1,Z22), (Ra2,Rb2,X1,Z23), (Ra2,Rb2,X1,Z24), (Ra2,Rb2,X1,Z25), (Ra2,Rb2,X1,Z26), (Ra2,Rb2,X1,Z27), (Ra2,Rb2,X1,Z28), (Ra2,Rb2,X1,Z29), (Ra2,Rb2,X1,Z30), (Ra2,Rb2,X1,Z31), (Ra2,Rb2,X1,Z32), (Ra2,Rb2,X1,Z33), (Ra2,Rb2,X1,Z34), (Ra2,Rb2,X1,Z35), (Ra2,Rb2,X1,Z36), (Ra2,Rb2,X1,Z37), (Ra2,Rb2,X1,Z38), (Ra2,Rb2,X1,Z39), (Ra2,Rb2,X2,Z1), (Ra2,Rb2,X2,Z2), (Ra2,Rb2,X2,Z3), (Ra2,Rb2,X2,Z4), (Ra2,Rb2,X2,Z5), (Ra2,Rb2,X2,Z6), (Ra2,Rb2,X2,Z7), (Ra2,Rb2,X2,Z8), (Ra2,Rb2,X2,Z9), (Ra2,Rb2,X2,Z10), (Ra2,Rb2,X2,Z11), (Ra2,Rb2,X2,Z12), (Ra2,Rb2,X2,Z13), (Ra2,Rb2,X2,Z14), (Ra2,Rb2,X2,Z15), (Ra2,Rb2,X2,Z16), (Ra2,Rb2,X2,Z17), (Ra2,Rb2,X2,Z18), (Ra2,Rb2,X2,Z19), (Ra2,Rb2,X2,Z20), (Ra2,Rb2,X2,Z21), (Ra2,Rb2,X2,Z22), (Ra2,Rb2,X2,Z23), (Ra2,Rb2,X2,Z24), (Ra2,Rb2,X2,Z25), (Ra2,Rb2,X2,Z26), (Ra2,Rb2,X2,Z27), (Ra2,Rb2,X2,Z28), (Ra2,Rb2,X2,Z29), (Ra2,Rb2,X2,Z30), (Ra2,Rb2,X2,Z31), (Ra2,Rb2,X2,Z32), (Ra2,Rb2,X2,Z33), (Ra2,Rb2,X2,Z34), (Ra2,Rb2,X2,Z35), (Ra2,Rb2,X2,Z36), (Ra2,Rb2,X2,Z37), (Ra2,Rb2,X2,Z38), (Ra2,Rb2,X2,Z39), (Ra2,Rb3,X1,Z1), (Ra2,Rb3,X1,Z2), (Ra2,Rb3,X1,Z3), (Ra2,Rb3,X1,Z4), (Ra2,Rb3,X1,Z5), (Ra2,Rb3,X1,Z6), (Ra2,Rb3,X1,Z7), (Ra2,Rb3,X1,Z8), (Ra2,Rb3,X1,Z9), (Ra2,Rb3,X1,Z10), (Ra2,Rb3,X1,Z11), (Ra2,Rb3,X1,Z12), (Ra2,Rb3,X1,Z13), (Ra2,Rb3,X1,Z14), (Ra2,Rb3,X1,Z15), (Ra2,Rb3,X1,Z16), (Ra2,Rb3,X1,Z17), (Ra2,Rb3,X1,Z18), (Ra2,Rb3,X1,Z19), (Ra2,Rb3,X1,Z20), (Ra2,Rb3,X1,Z21), (Ra2,Rb3,X1,Z22), (Ra2,Rb3,X1,Z23), (Ra2,Rb3,X1,Z24), (Ra2,Rb3,X1,Z25), (Ra2,Rb3,X1,Z26), (Ra2,Rb3,X1,Z27), (Ra2,Rb3,X1,Z28), (Ra2,Rb3,X1,Z29), (Ra2,Rb3,X1,Z30), (Ra2,Rb3,X1,Z31), (Ra2,Rb3,X1,Z32), (Ra2,Rb3,X1,Z33), (Ra2,Rb3,X1,Z34), (Ra2,Rb3,X1,Z35), (Ra2,Rb3,X1,Z36), (Ra2,Rb3,X1,Z37), (Ra2,Rb3,X1,Z38), (Ra2,Rb3,X1,Z39), (Ra2,Rb3,X2,Z1), (Ra2,Rb3,X2,Z2), (Ra2,Rb3,X2,Z3), (Ra2,Rb3,X2,Z4), (Ra2,Rb3,X2,Z5), (Ra2,Rb3,X2,Z6), (Ra2,Rb3,X2,Z7), (Ra2,Rb3,X2,Z8), (Ra2,Rb3,X2,Z9), (Ra2,Rb3,X2,Z10), (Ra2,Rb3,X2,Z11), (Ra2,Rb3,X2,Z12), (Ra2,Rb3,X2,Z13), (Ra2,Rb3,X2,Z14), (Ra2,Rb3,X2,Z15), (Ra2,Rb3,X2,Z16), (Ra2,Rb3,X2,Z17), (Ra2,Rb3,X2,Z18), (Ra2,Rb3,X2,Z19), (Ra2,Rb3,X2,Z20), (Ra2,Rb3,X2,Z21), (Ra2,Rb3,X2,Z22), (Ra2,Rb3,X2,Z23), (Ra2,Rb3,X2,Z24), (Ra2,Rb3,X2,Z25), (Ra2,Rb3,X2,Z26), (Ra2,Rb3,X2,Z27), (Ra2,Rb3,X2,Z28), (Ra2,Rb3,X2,Z29), (Ra2,Rb3,X2,Z30), (Ra2,Rb3,X2,Z31), (Ra2,Rb3,X2,Z32), (Ra2,Rb3,X2,Z33), (Ra2,Rb3,X2,Z34), (Ra2,Rb3,X2,Z35), (Ra2,Rb3,X2,Z36), (Ra2,Rb3,X2,Z37), (Ra2,Rb3,X2,Z38), (Ra2,Rb3,X2,Z39), (Ra2,Rb4,X1,Z1), (Ra2,Rb4,X1,Z2), (Ra2,Rb4,X1,Z3), (Ra2,Rb4,X1,Z4), (Ra2,Rb4,X1,Z5), (Ra2,Rb4,X1,Z6), (Ra2,Rb4,X1,Z7), (Ra2,Rb4,X1,Z8), (Ra2,Rb4,X1,Z9), (Ra2,Rb4,X1,Z10), (Ra2,Rb4,X1,Z11), (Ra2,Rb4,X1,Z12), (Ra2,Rb4,X1,Z13), (Ra2,Rb4,X1,Z14), (Ra2,Rb4,X1,Z15), (Ra2,Rb4,X1,Z16), (Ra2,Rb4,X1,Z17), (Ra2,Rb4,X1,Z18), (Ra2,Rb4,X1,Z19), (Ra2,Rb4,X1,Z20), (Ra2,Rb4,X1,Z21), (Ra2,Rb4,X1,Z22), (Ra2,Rb4,X1,Z23), (Ra2,Rb4,X1,Z24), (Ra2,Rb4,X1,Z25), (Ra2,Rb4,X1,Z26), (Ra2,Rb4,X1,Z27), (Ra2,Rb4,X1,Z28), (Ra2,Rb4,X1,Z29), (Ra2,Rb4,X1,Z30), (Ra2,Rb4,X1,Z31), (Ra2,Rb4,X1,Z32), (Ra2,Rb4,X1,Z33), (Ra2,Rb4,X1,Z34), (Ra2,Rb4,X1,Z35), (Ra2,Rb4,X1,Z36), (Ra2,Rb4,X1,Z37), (Ra2,Rb4,X1,Z38), (Ra2,Rb4,X1,Z39), (Ra2,Rb4,X2,Z1), (Ra2,Rb4,X2,Z2), (Ra2,Rb4,X2,Z3), (Ra2,Rb4,X2,Z4), (Ra2,Rb4,X2,Z5), (Ra2,Rb4,X2,Z6), (Ra2,Rb4,X2,Z7), (Ra2,Rb4,X2,Z8), (Ra2,Rb4,X2,Z9), (Ra2,Rb4,X2,Z10), (Ra2,Rb4,X2,Z11), (Ra2,Rb4,X2,Z12), (Ra2,Rb4,X2,Z13), (Ra2,Rb4,X2,Z14), (Ra2,Rb4,X2,Z15), (Ra2,Rb4,X2,Z16), (Ra2,Rb4,X2,Z17), (Ra2,Rb4,X2,Z18), (Ra2,Rb4,X2,Z19), (Ra2,Rb4,X2,Z20), (Ra2,Rb4,X2,Z21), (Ra2,Rb4,X2,Z22), (Ra2,Rb4,X2,Z23), (Ra2,Rb4,X2,Z24), (Ra2,Rb4,X2,Z25), (Ra2,Rb4,X2,Z26), (Ra2,Rb4,X2,Z27), (Ra2,Rb4,X2,Z28), (Ra2,Rb4,X2,Z29), (Ra2,Rb4,X2,Z30), (Ra2,Rb4,X2,Z31), (Ra2,Rb4,X2,Z32), (Ra2,Rb4,X2,Z33), (Ra2,Rb4,X2,Z34), (Ra2,Rb4,X2,Z35), (Ra2,Rb4,X2,Z36), (Ra2,Rb4,X2,Z37), (Ra2,Rb4,X2,Z38), (Ra2,Rb4,X2,Z39), (Ra2,Rb5,X1,Z1), (Ra2,Rb5,X1,Z2), (Ra2,Rb5,X1,Z3), (Ra2,Rb5,X1,Z4), (Ra2,Rb5,X1,Z5), (Ra2,Rb5,X1,Z6), (Ra2,Rb5,X1,Z7), (Ra2,Rb5,X1,Z8), (Ra2,Rb5,X1,Z9), (Ra2,Rb5,X1,Z10), (Ra2,Rb5,X1,Z11), (Ra2,Rb5,X1,Z12), (Ra2,Rb5,X1,Z13), (Ra2,Rb5,X1,Z14), (Ra2,Rb5,X1,Z15), (Ra2,Rb5,X1,Z16), (Ra2,Rb5,X1,Z17), (Ra2,Rb5,X1,Z18), (Ra2,Rb5,X1,Z19), (Ra2,Rb5,X1,Z20), (Ra2,Rb5,X1,Z21), (Ra2,Rb5,X1,Z22), (Ra2,Rb5,X1,Z23), (Ra2,Rb5,X1,Z24), (Ra2,Rb5,X1,Z25), (Ra2,Rb5,X1,Z26), (Ra2,Rb5,X1,Z27), (Ra2,Rb5,X1,Z28), (Ra2,Rb5,X1,Z29), (Ra2,Rb5,X1,Z30), (Ra2,Rb5,X1,Z31), (Ra2,Rb5,X1,Z32), (Ra2,Rb5,X1,Z33), (Ra2,Rb5,X1,Z34), (Ra2,Rb5,X1,Z35), (Ra2,Rb5,X1,Z36), (Ra2,Rb5,X1,Z37), (Ra2,Rb5,X1,Z38), (Ra2,Rb5,X1,Z39), (Ra2,Rb5,X2,Z1), (Ra2,Rb5,X2,Z2), (Ra2,Rb5,X2,Z3), (Ra2,Rb5,X2,Z4), (Ra2,Rb5,X2,Z5), (Ra2,Rb5,X2,Z6), (Ra2,Rb5,X2,Z7), (Ra2,Rb5,X2,Z8), (Ra2,Rb5,X2,Z9), (Ra2,Rb5,X2,Z10), (Ra2,Rb5,X2,Z11), (Ra2,Rb5,X2,Z12), (Ra2,Rb5,X2,Z13), (Ra2,Rb5,X2,Z14), (Ra2,Rb5,X2,Z15), (Ra2,Rb5,X2,Z16), (Ra2,Rb5,X2,Z17), (Ra2,Rb5,X2,Z18), (Ra2,Rb5,X2,Z19), (Ra2,Rb5,X2,Z20), (Ra2,Rb5,X2,Z21), (Ra2,Rb5,X2,Z22), (Ra2,Rb5,X2,Z23), (Ra2,Rb5,X2,Z24), (Ra2,Rb5,X2,Z25), (Ra2,Rb5,X2,Z26), (Ra2,Rb5,X2,Z27), (Ra2,Rb5,X2,Z28), (Ra2,Rb5,X2,Z29), (Ra2,Rb5,X2,Z30), (Ra2,Rb5,X2,Z31), (Ra2,Rb5,X2,Z32), (Ra2,Rb5,X2,Z33), (Ra2,Rb5,X2,Z34), (Ra2,Rb5,X2,Z35), (Ra2,Rb5,X2,Z36), (Ra2,Rb5,X2,Z37), (Ra2,Rb5,X2,Z38), (Ra2,Rb5,X2,Z39), (Ra2,Rb6,X1,Z1), (Ra2,Rb6,X1,Z2), (Ra2,Rb6,X1,Z3), (Ra2,Rb6,X1,Z4), (Ra2,Rb6,X1,Z5), (Ra2,Rb6,X1,Z6), (Ra2,Rb6,X1,Z7), (Ra2,Rb6,X1,Z8), (Ra2,Rb6,X1,Z9), (Ra2,Rb6,X1,Z10), (Ra2,Rb6,X1,Z11), (Ra2,Rb6,X1,Z12), (Ra2,Rb6,X1,Z13), (Ra2,Rb6,X1,Z14), (Ra2,Rb6,X1,Z15), (Ra2,Rb6,X1,Z16), (Ra2,Rb6,X1,Z17), (Ra2,Rb6,X1,Z18), (Ra2,Rb6,X1,Z19), (Ra2,Rb6,X1,Z20), (Ra2,Rb6,X1,Z21), (Ra2,Rb6,X1,Z22), (Ra2,Rb6,X1,Z23), (Ra2,Rb6,X1,Z24), (Ra2,Rb6,X1,Z25), (Ra2,Rb6,X1,Z26), (Ra2,Rb6,X1,Z27), (Ra2,Rb6,X1,Z28), (Ra2,Rb6,X1,Z29), (Ra2,Rb6,X1,Z30), (Ra2,Rb6,X1,Z31), (Ra2,Rb6,X1,Z32), (Ra2,Rb6,X1,Z33), (Ra2,Rb6,X1,Z34), (Ra2,Rb6,X1,Z35), (Ra2,Rb6,X1,Z36), (Ra2,Rb6,X1,Z37), (Ra2,Rb6,X1,Z38), (Ra2,Rb6,X1,Z39), (Ra2,Rb6,X2,Z1), (Ra2,Rb6,X2,Z2), (Ra2,Rb6,X2,Z3), (Ra2,Rb6,X2,Z4), (Ra2,Rb6,X2,Z5), (Ra2,Rb6,X2,Z6), (Ra2,Rb6,X2,Z7), (Ra2,Rb6,X2,Z8), (Ra2,Rb6,X2,Z9), (Ra2,Rb6,X2,Z10), (Ra2,Rb6,X2,Z11), (Ra2,Rb6,X2,Z12), (Ra2,Rb6,X2,Z13), (Ra2,Rb6,X2,Z14), (Ra2,Rb6,X2,Z15), (Ra2,Rb6,X2,Z16), (Ra2,Rb6,X2,Z17), (Ra2,Rb6,X2,Z18), (Ra2,Rb6,X2,Z19), (Ra2,Rb6,X2,Z20), (Ra2,Rb6,X2,Z21), (Ra2,Rb6,X2,Z22), (Ra2,Rb6,X2,Z23), (Ra2,Rb6,X2,Z24), (Ra2,Rb6,X2,Z25), (Ra2,Rb6,X2,Z26), (Ra2,Rb6,X2,Z27), (Ra2,Rb6,X2,Z28), (Ra2,Rb6,X2,Z29), (Ra2,Rb6,X2,Z30), (Ra2,Rb6,X2,Z31), (Ra2,Rb6,X2,Z32), (Ra2,Rb6,X2,Z33), (Ra2,Rb6,X2,Z34), (Ra2,Rb6,X2,Z35), (Ra2,Rb6,X2,Z36), (Ra2,Rb6,X2,Z37), (Ra2,Rb6,X2,Z38), (Ra2,Rb6,X2,Z39), (Ra2,Rb7,X1,Z1), (Ra2,Rb7,X1,Z2), (Ra2,Rb7,X1,Z3), (Ra2,Rb7,X1,Z4), (Ra2,Rb7,X1,Z5), (Ra2,Rb7,X1,Z6), (Ra2,Rb7,X1,Z7), (Ra2,Rb7,X1,Z8), (Ra2,Rb7,X1,Z9), (Ra2,Rb7,X1,Z10), (Ra2,Rb7,X1,Z11), (Ra2,Rb7,X1,Z12), (Ra2,Rb7,X1,Z13), (Ra2,Rb7,X1,Z14), (Ra2,Rb7,X1,Z15), (Ra2,Rb7,X1,Z16), (Ra2,Rb7,X1,Z17), (Ra2,Rb7,X1,Z18), (Ra2,Rb7,X1,Z19), (Ra2,Rb7,X1,Z20), (Ra2,Rb7,X1,Z21), (Ra2,Rb7,X1,Z22), (Ra2,Rb7,X1,Z23), (Ra2,Rb7,X1,Z24), (Ra2,Rb7,X1,Z25), (Ra2,Rb7,X1,Z26), (Ra2,Rb7,X1,Z27), 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(Ra2,Rb8,X1,Z6), (Ra2,Rb8,X1,Z7), (Ra2,Rb8,X1,Z8), (Ra2,Rb8,X1,Z9), (Ra2,Rb8,X1,Z10), (Ra2,Rb8,X1,Z11), (Ra2,Rb8,X1,Z12), (Ra2,Rb8,X1,Z13), (Ra2,Rb8,X1,Z14), (Ra2,Rb8,X1,Z15), (Ra2,Rb8,X1,Z16), (Ra2,Rb8,X1,Z17), (Ra2,Rb8,X1,Z18), (Ra2,Rb8,X1,Z19), (Ra2,Rb8,X1,Z20), (Ra2,Rb8,X1,Z21), (Ra2,Rb8,X1,Z22), (Ra2,Rb8,X1,Z23), (Ra2,Rb8,X1,Z24), (Ra2,Rb8,X1,Z25), (Ra2,Rb8,X1,Z26), (Ra2,Rb8,X1,Z27), (Ra2,Rb8,X1,Z28), (Ra2,Rb8,X1,Z29), (Ra2,Rb8,X1,Z30), (Ra2,Rb8,X1,Z31), (Ra2,Rb8,X1,Z32), (Ra2,Rb8,X1,Z33), (Ra2,Rb8,X1,Z34), (Ra2,Rb8,X1,Z35), (Ra2,Rb8,X1,Z36), (Ra2,Rb8,X1,Z37), (Ra2,Rb8,X1,Z38), (Ra2,Rb8,X1,Z39), (Ra2,Rb8,X2,Z1), (Ra2,Rb8,X2,Z2), (Ra2,Rb8,X2,Z3), (Ra2,Rb8,X2,Z4), (Ra2,Rb8,X2,Z5), (Ra2,Rb8,X2,Z6), (Ra2,Rb8,X2,Z7), (Ra2,Rb8,X2,Z8), (Ra2,Rb8,X2,Z9), (Ra2,Rb8,X2,Z10), (Ra2,Rb8,X2,Z11), (Ra2,Rb8,X2,Z12), (Ra2,Rb8,X2,Z13), (Ra2,Rb8,X2,Z14), (Ra2,Rb8,X2,Z15), (Ra2,Rb8,X2,Z16), (Ra2,Rb8,X2,Z17), (Ra2,Rb8,X2,Z18), (Ra2,Rb8,X2,Z19), (Ra2,Rb8,X2,Z20), (Ra2,Rb8,X2,Z21), (Ra2,Rb8,X2,Z22), 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(Ra3,Rb1,X2,Z1), (Ra3,Rb1,X2,Z2), (Ra3,Rb1,X2,Z3), (Ra3,Rb1,X2,Z4), (Ra3,Rb1,X2,Z5), (Ra3,Rb1,X2,Z6), (Ra3,Rb1,X2,Z7), (Ra3,Rb1,X2,Z8), (Ra3,Rb1,X2,Z9), (Ra3,Rb1,X2,Z10), (Ra3,Rb1,X2,Z11), (Ra3,Rb1,X2,Z12), (Ra3,Rb1,X2,Z13), (Ra3,Rb1,X2,Z14), (Ra3,Rb1,X2,Z15), (Ra3,Rb1,X2,Z16), (Ra3,Rb1,X2,Z17), (Ra3,Rb1,X2,Z18), (Ra3,Rb1,X2,Z19), (Ra3,Rb1,X2,Z20), (Ra3,Rb1,X2,Z21), (Ra3,Rb1,X2,Z22), (Ra3,Rb1,X2,Z23), (Ra3,Rb1,X2,Z24), (Ra3,Rb1,X2,Z25), (Ra3,Rb1,X2,Z26), (Ra3,Rb1,X2,Z27), (Ra3,Rb1,X2,Z28), (Ra3,Rb1,X2,Z29), (Ra3,Rb1,X2,Z30), (Ra3,Rb1,X2,Z31), (Ra3,Rb1,X2,Z32), (Ra3,Rb1,X2,Z33), (Ra3,Rb1,X2,Z34), (Ra3,Rb1,X2,Z35), (Ra3,Rb1,X2,Z36), (Ra3,Rb1,X2,Z37), (Ra3,Rb1,X2,Z38), (Ra3,Rb1,X2,Z39), (Ra3,Rb2,X1,Z1), (Ra3,Rb2,X1,Z2), (Ra3,Rb2,X1,Z3), (Ra3,Rb2,X1,Z4), (Ra3,Rb2,X1,Z5), (Ra3,Rb2,X1,Z6), (Ra3,Rb2,X1,Z7), (Ra3,Rb2,X1,Z8), (Ra3,Rb2,X1,Z9), (Ra3,Rb2,X1,Z10), (Ra3,Rb2,X1,Z11), (Ra3,Rb2,X1,Z12), (Ra3,Rb2,X1,Z13), (Ra3,Rb2,X1,Z14), (Ra3,Rb2,X1,Z15), (Ra3,Rb2,X1,Z16), (Ra3,Rb2,X1,Z17), 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(Ra3,Rb5,X1,Z8), (Ra3,Rb5,X1,Z9), (Ra3,Rb5,X1,Z10), (Ra3,Rb5,X1,Z11), (Ra3,Rb5,X1,Z12), (Ra3,Rb5,X1,Z13), (Ra3,Rb5,X1,Z14), (Ra3,Rb5,X1,Z15), (Ra3,Rb5,X1,Z16), (Ra3,Rb5,X1,Z17), (Ra3,Rb5,X1,Z18), (Ra3,Rb5,X1,Z19), (Ra3,Rb5,X1,Z20), (Ra3,Rb5,X1,Z21), (Ra3,Rb5,X1,Z22), (Ra3,Rb5,X1,Z23), (Ra3,Rb5,X1,Z24), (Ra3,Rb5,X1,Z25), (Ra3,Rb5,X1,Z26), (Ra3,Rb5,X1,Z27), (Ra3,Rb5,X1,Z28), (Ra3,Rb5,X1,Z29), (Ra3,Rb5,X1,Z30), (Ra3,Rb5,X1,Z31), (Ra3,Rb5,X1,Z32), (Ra3,Rb5,X1,Z33), (Ra3,Rb5,X1,Z34), (Ra3,Rb5,X1,Z35), (Ra3,Rb5,X1,Z36), (Ra3,Rb5,X1,Z37), (Ra3,Rb5,X1,Z38), (Ra3,Rb5,X1,Z39), (Ra3,Rb5,X2,Z1), (Ra3,Rb5,X2,Z2), (Ra3,Rb5,X2,Z3), (Ra3,Rb5,X2,Z4), (Ra3,Rb5,X2,Z5), (Ra3,Rb5,X2,Z6), (Ra3,Rb5,X2,Z7), (Ra3,Rb5,X2,Z8), (Ra3,Rb5,X2,Z9), (Ra3,Rb5,X2,Z10), (Ra3,Rb5,X2,Z11), (Ra3,Rb5,X2,Z12), (Ra3,Rb5,X2,Z13), (Ra3,Rb5,X2,Z14), (Ra3,Rb5,X2,Z15), (Ra3,Rb5,X2,Z16), (Ra3,Rb5,X2,Z17), (Ra3,Rb5,X2,Z18), (Ra3,Rb5,X2,Z19), (Ra3,Rb5,X2,Z20), (Ra3,Rb5,X2,Z21), (Ra3,Rb5,X2,Z22), (Ra3,Rb5,X2,Z23), (Ra3,Rb5,X2,Z24), 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(Ra3,Rb6,X2,Z3), (Ra3,Rb6,X2,Z4), (Ra3,Rb6,X2,Z5), (Ra3,Rb6,X2,Z6), (Ra3,Rb6,X2,Z7), (Ra3,Rb6,X2,Z8), (Ra3,Rb6,X2,Z9), (Ra3,Rb6,X2,Z10), (Ra3,Rb6,X2,Z11), (Ra3,Rb6,X2,Z12), (Ra3,Rb6,X2,Z13), (Ra3,Rb6,X2,Z14), (Ra3,Rb6,X2,Z15), (Ra3,Rb6,X2,Z16), (Ra3,Rb6,X2,Z17), (Ra3,Rb6,X2,Z18), (Ra3,Rb6,X2,Z19), (Ra3,Rb6,X2,Z20), (Ra3,Rb6,X2,Z21), (Ra3,Rb6,X2,Z22), (Ra3,Rb6,X2,Z23), (Ra3,Rb6,X2,Z24), (Ra3,Rb6,X2,Z25), (Ra3,Rb6,X2,Z26), (Ra3,Rb6,X2,Z27), (Ra3,Rb6,X2,Z28), (Ra3,Rb6,X2,Z29), (Ra3,Rb6,X2,Z30), (Ra3,Rb6,X2,Z31), (Ra3,Rb6,X2,Z32), (Ra3,Rb6,X2,Z33), (Ra3,Rb6,X2,Z34), (Ra3,Rb6,X2,Z35), (Ra3,Rb6,X2,Z36), (Ra3,Rb6,X2,Z37), (Ra3,Rb6,X2,Z38), (Ra3,Rb6,X2,Z39), (Ra3,Rb7,X1,Z1), (Ra3,Rb7,X1,Z2), (Ra3,Rb7,X1,Z3), (Ra3,Rb7,X1,Z4), (Ra3,Rb7,X1,Z5), (Ra3,Rb7,X1,Z6), (Ra3,Rb7,X1,Z7), (Ra3,Rb7,X1,Z8), (Ra3,Rb7,X1,Z9), (Ra3,Rb7,X1,Z10), (Ra3,Rb7,X1,Z11), (Ra3,Rb7,X1,Z12), (Ra3,Rb7,X1,Z13), (Ra3,Rb7,X1,Z14), (Ra3,Rb7,X1,Z15), (Ra3,Rb7,X1,Z16), (Ra3,Rb7,X1,Z17), (Ra3,Rb7,X1,Z18), (Ra3,Rb7,X1,Z19), 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(Ra3,Rb7,X2,Z37), (Ra3,Rb7,X2,Z38), (Ra3,Rb7,X2,Z39), (Ra3,Rb8,X1,Z1), (Ra3,Rb8,X1,Z2), (Ra3,Rb8,X1,Z3), (Ra3,Rb8,X1,Z4), (Ra3,Rb8,X1,Z5), (Ra3,Rb8,X1,Z6), (Ra3,Rb8,X1,Z7), (Ra3,Rb8,X1,Z8), (Ra3,Rb8,X1,Z9), (Ra3,Rb8,X1,Z10), (Ra3,Rb8,X1,Z11), (Ra3,Rb8,X1,Z12), (Ra3,Rb8,X1,Z13), (Ra3,Rb8,X1,Z14), (Ra3,Rb8,X1,Z15), (Ra3,Rb8,X1,Z16), (Ra3,Rb8,X1,Z17), (Ra3,Rb8,X1,Z18), (Ra3,Rb8,X1,Z19), (Ra3,Rb8,X1,Z20), (Ra3,Rb8,X1,Z21), (Ra3,Rb8,X1,Z22), (Ra3,Rb8,X1,Z23), (Ra3,Rb8,X1,Z24), (Ra3,Rb8,X1,Z25), (Ra3,Rb8,X1,Z26), (Ra3,Rb8,X1,Z27), (Ra3,Rb8,X1,Z28), (Ra3,Rb8,X1,Z29), (Ra3,Rb8,X1,Z30), (Ra3,Rb8,X1,Z31), (Ra3,Rb8,X1,Z32), (Ra3,Rb8,X1,Z33), (Ra3,Rb8,X1,Z34), (Ra3,Rb8,X1,Z35), (Ra3,Rb8,X1,Z36), (Ra3,Rb8,X1,Z37), (Ra3,Rb8,X1,Z38), (Ra3,Rb8,X1,Z39), (Ra3,Rb8,X2,Z1), (Ra3,Rb8,X2,Z2), (Ra3,Rb8,X2,Z3), (Ra3,Rb8,X2,Z4), (Ra3,Rb8,X2,Z5), (Ra3,Rb8,X2,Z6), (Ra3,Rb8,X2,Z7), (Ra3,Rb8,X2,Z8), (Ra3,Rb8,X2,Z9), (Ra3,Rb8,X2,Z10), (Ra3,Rb8,X2,Z11), (Ra3,Rb8,X2,Z12), (Ra3,Rb8,X2,Z13), (Ra3,Rb8,X2,Z14), 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(Ra4,Rb3,X2,Z5), (Ra4,Rb3,X2,Z6), (Ra4,Rb3,X2,Z7), (Ra4,Rb3,X2,Z8), (Ra4,Rb3,X2,Z9), (Ra4,Rb3,X2,Z10), (Ra4,Rb3,X2,Z11), (Ra4,Rb3,X2,Z12), (Ra4,Rb3,X2,Z13), (Ra4,Rb3,X2,Z14), (Ra4,Rb3,X2,Z15), (Ra4,Rb3,X2,Z16), (Ra4,Rb3,X2,Z17), (Ra4,Rb3,X2,Z18), (Ra4,Rb3,X2,Z19), (Ra4,Rb3,X2,Z20), (Ra4,Rb3,X2,Z21), (Ra4,Rb3,X2,Z22), (Ra4,Rb3,X2,Z23), (Ra4,Rb3,X2,Z24), (Ra4,Rb3,X2,Z25), (Ra4,Rb3,X2,Z26), (Ra4,Rb3,X2,Z27), (Ra4,Rb3,X2,Z28), (Ra4,Rb3,X2,Z29), (Ra4,Rb3,X2,Z30), (Ra4,Rb3,X2,Z31), (Ra4,Rb3,X2,Z32), (Ra4,Rb3,X2,Z33), (Ra4,Rb3,X2,Z34), (Ra4,Rb3,X2,Z35), (Ra4,Rb3,X2,Z36), (Ra4,Rb3,X2,Z37), (Ra4,Rb3,X2,Z38), (Ra4,Rb3,X2,Z39), (Ra4,Rb4,X1,Z1), (Ra4,Rb4,X1,Z2), (Ra4,Rb4,X1,Z3), (Ra4,Rb4,X1,Z4), (Ra4,Rb4,X1,Z5), (Ra4,Rb4,X1,Z6), (Ra4,Rb4,X1,Z7), (Ra4,Rb4,X1,Z8), (Ra4,Rb4,X1,Z9), (Ra4,Rb4,X1,Z10), (Ra4,Rb4,X1,Z11), (Ra4,Rb4,X1,Z12), (Ra4,Rb4,X1,Z13), (Ra4,Rb4,X1,Z14), (Ra4,Rb4,X1,Z15), (Ra4,Rb4,X1,Z16), (Ra4,Rb4,X1,Z17), (Ra4,Rb4,X1,Z18), (Ra4,Rb4,X1,Z19), (Ra4,Rb4,X1,Z20), (Ra4,Rb4,X1,Z21), (Ra4,Rb4,X1,Z22), (Ra4,Rb4,X1,Z23), (Ra4,Rb4,X1,Z24), (Ra4,Rb4,X1,Z25), (Ra4,Rb4,X1,Z26), (Ra4,Rb4,X1,Z27), (Ra4,Rb4,X1,Z28), (Ra4,Rb4,X1,Z29), (Ra4,Rb4,X1,Z30), (Ra4,Rb4,X1,Z31), (Ra4,Rb4,X1,Z32), (Ra4,Rb4,X1,Z33), (Ra4,Rb4,X1,Z34), (Ra4,Rb4,X1,Z35), (Ra4,Rb4,X1,Z36), (Ra4,Rb4,X1,Z37), (Ra4,Rb4,X1,Z38), (Ra4,Rb4,X1,Z39), (Ra4,Rb4,X2,Z1), (Ra4,Rb4,X2,Z2), (Ra4,Rb4,X2,Z3), (Ra4,Rb4,X2,Z4), (Ra4,Rb4,X2,Z5), (Ra4,Rb4,X2,Z6), (Ra4,Rb4,X2,Z7), (Ra4,Rb4,X2,Z8), (Ra4,Rb4,X2,Z9), (Ra4,Rb4,X2,Z10), (Ra4,Rb4,X2,Z11), (Ra4,Rb4,X2,Z12), (Ra4,Rb4,X2,Z13), (Ra4,Rb4,X2,Z14), (Ra4,Rb4,X2,Z15), (Ra4,Rb4,X2,Z16), (Ra4,Rb4,X2,Z17), (Ra4,Rb4,X2,Z18), (Ra4,Rb4,X2,Z19), (Ra4,Rb4,X2,Z20), (Ra4,Rb4,X2,Z21), (Ra4,Rb4,X2,Z22), (Ra4,Rb4,X2,Z23), (Ra4,Rb4,X2,Z24), (Ra4,Rb4,X2,Z25), (Ra4,Rb4,X2,Z26), (Ra4,Rb4,X2,Z27), (Ra4,Rb4,X2,Z28), (Ra4,Rb4,X2,Z29), (Ra4,Rb4,X2,Z30), (Ra4,Rb4,X2,Z31), (Ra4,Rb4,X2,Z32), (Ra4,Rb4,X2,Z33), (Ra4,Rb4,X2,Z34), (Ra4,Rb4,X2,Z35), (Ra4,Rb4,X2,Z36), (Ra4,Rb4,X2,Z37), (Ra4,Rb4,X2,Z38), (Ra4,Rb4,X2,Z39), (Ra4,Rb5,X1,Z1), (Ra4,Rb5,X1,Z2), (Ra4,Rb5,X1,Z3), (Ra4,Rb5,X1,Z4), (Ra4,Rb5,X1,Z5), (Ra4,Rb5,X1,Z6), (Ra4,Rb5,X1,Z7), (Ra4,Rb5,X1,Z8), (Ra4,Rb5,X1,Z9), (Ra4,Rb5,X1, Z10), (Ra4,Rb5,X1,Z11), (Ra4,Rb5,X1,Z12), (Ra4,Rb5,X1,Z13), (Ra4,Rb5,X1,Z14), (Ra4,Rb5,X1,Z15), (Ra4,Rb5,X1,Z16), (Ra4,Rb5,X1,Z17), (Ra4,Rb5,X1,Z18), (Ra4,Rb5,X1,Z19), (Ra4,Rb5,X1,Z20), (Ra4,Rb5,X1,Z21), (Ra4,Rb5,X1,Z22), (Ra4,Rb5,X1,Z23), (Ra4,Rb5,X1,Z24), (Ra4,Rb5,X1,Z25), (Ra4,Rb5,X1,Z26), (Ra4,Rb5,X1,Z27), (Ra4,Rb5,X1,Z28), (Ra4,Rb5,X1,Z29), (Ra4,Rb5,X1,Z30), (Ra4,Rb5,X1,Z31), (Ra4,Rb5,X1,Z32), (Ra4,Rb5,X1,Z33), (Ra4,Rb5,X1,Z34), (Ra4,Rb5,X1,Z35), (Ra4,Rb5,X1,Z36), (Ra4,Rb5,X1,Z37), (Ra4,Rb5,X1,Z38), (Ra4,Rb5,X1,Z39), (Ra4,Rb5,X2,Z1), (Ra4,Rb5,X2,Z2), (Ra4,Rb5,X2,Z3), (Ra4,Rb5,X2,Z4), (Ra4,Rb5,X2,Z5), (Ra4,Rb5,X2,Z6), (Ra4,Rb5,X2,Z7), (Ra4,Rb5,X2,Z8), (Ra4,Rb5,X2,Z9), (Ra4,Rb5,X2,Z10), (Ra4,Rb5,X2,Z11), (Ra4,Rb5,X2,Z12), (Ra4,Rb5,X2,Z13), (Ra4,Rb5,X2,Z14), (Ra4,Rb5,X2,Z15), (Ra4,Rb5,X2,Z16), 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(Ra4,Rb6,X1,Z34), (Ra4,Rb6,X1,Z35), (Ra4,Rb6,X1,Z36), (Ra4,Rb6,X1,Z37), (Ra4,Rb6,X1,Z38), (Ra4,Rb6,X1,Z39), (Ra4,Rb6,X2,Z1), (Ra4,Rb6,X2,Z2), (Ra4,Rb6,X2,Z3), (Ra4,Rb6,X2,Z4), (Ra4,Rb6,X2,Z5), (Ra4,Rb6,X2,Z6), (Ra4,Rb6,X2,Z7), (Ra4,Rb6,X2,Z8), (Ra4,Rb6,X2,Z9), (Ra4,Rb6,X2,Z10), (Ra4,Rb6,X2,Z11), (Ra4,Rb6,X2,Z12), (Ra4,Rb6,X2,Z13), (Ra4,Rb6,X2,Z14), (Ra4,Rb6,X2,Z15), (Ra4,Rb6,X2,Z16), (Ra4,Rb6,X2,Z17), (Ra4,Rb6,X2,Z 18), (Ra4,Rb6,X2,Z19), (Ra4,Rb6,X2,Z20), (Ra4,Rb6,X2,Z21), (Ra4,Rb6,X2,Z22), (Ra4,Rb6,X2,Z23), (Ra4,Rb6,X2,Z24), (Ra4,Rb6,X2,Z25), (Ra4,Rb6,X2,Z26), (Ra4,Rb6,X2,Z27), (Ra4,Rb6,X2,Z28), (Ra4,Rb6,X2,Z29), (Ra4,Rb6,X2,Z30), (Ra4,Rb6,X2,Z31), (Ra4,Rb6,X2,Z32), (Ra4,Rb6,X2,Z33), (Ra4,Rb6,X2,Z34), (Ra4,Rb6,X2,Z35), (Ra4,Rb6,X2,Z36), (Ra4,Rb6,X2,Z37), (Ra4,Rb6,X2,Z38), (Ra4,Rb6,X2,Z39), (Ra4,Rb7,X1,Z1), (Ra4,Rb7,X1,Z2), (Ra4,Rb7,X1,Z3), (Ra4,Rb7,X1,Z4), (Ra4,Rb7,X1,Z5), (Ra4,Rb7,X1,Z6), (Ra4,Rb7,X1,Z7), (Ra4,Rb7,X1,Z8), (Ra4,Rb7,X1,Z9), (Ra4,Rb7,X1,Z10), (Ra4,Rb7,X1,Z11), 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(Ra5,Rb2,X1,Z2), (Ra5,Rb2,X1,Z3), (Ra5,Rb2,X1,Z4), (Ra5,Rb2,X1,Z5), (Ra5,Rb2,X1,Z6), (Ra5,Rb2,X1,Z7), (Ra5,Rb2,X1,Z8), (Ra5,Rb2,X1,Z9), (Ra5,Rb2,X1,Z10), (Ra5,Rb2,X1,Z11), (Ra5,Rb2,X1,Z12), (Ra5,Rb2,X1,Z13), (Ra5,Rb2,X1,Z14), (Ra5,Rb2,X1,Z15), (Ra5,Rb2,X1,Z16), (Ra5,Rb2,X1,Z17), (Ra5,Rb2,X1,Z18), (Ra5,Rb2,X1,Z19), (Ra5,Rb2,X1,Z20), (Ra5,Rb2,X1,Z21), (Ra5,Rb2,X1,Z22), (Ra5,Rb2,X1,Z23), (Ra5,Rb2,X1,Z24), (Ra5,Rb2,X1,Z25), (Ra5,Rb2,X1,Z26), (Ra5,Rb2,X1,Z27), (Ra5,Rb2,X1,Z28), (Ra5,Rb2,X1,Z29), (Ra5,Rb2,X1,Z30), (Ra5,Rb2,X1,Z31), (Ra5,Rb2,X1,Z32), (Ra5,Rb2,X1,Z33), (Ra5,Rb2,X1,Z34), (Ra5,Rb2,X1,Z35), (Ra5,Rb2,X1,Z36), (Ra5,Rb2,X1,Z37), (Ra5,Rb2,X1,Z38), (Ra5,Rb2,X1,Z39), (Ra5,Rb2,X2,Z1), (Ra5,Rb2,X2,Z2), (Ra5,Rb2,X2,Z3), (Ra5,Rb2,X2,Z4), (Ra5,Rb2,X2,Z5), (Ra5,Rb2,X2,Z6), (Ra5,Rb2,X2,Z7), (Ra5,Rb2,X2,Z8), (Ra5,Rb2,X2,Z9), (Ra5,Rb2,X2,Z10), (Ra5,Rb2,X2,Z11), (Ra5,Rb2,X2,Z12), (Ra5,Rb2,X2,Z13), (Ra5,Rb2,X2,Z14), (Ra5,Rb2,X2,Z15), (Ra5,Rb2,X2,Z16), (Ra5,Rb2,X2,Z17), (Ra5,Rb2,X2,Z18), (Ra5,Rb2,X2,Z19), (Ra5,Rb2,X2,Z20), (Ra5,Rb2,X2,Z21), (Ra5,Rb2,X2,Z22), (Ra5,Rb2,X2,Z23), (Ra5,Rb2,X2,Z24), (Ra5,Rb2,X2,Z25), (Ra5,Rb2,X2,Z26), (Ra5,Rb2,X2,Z27), (Ra5,Rb2,X2,Z28), (Ra5,Rb2,X2,Z29), (Ra5,Rb2,X2,Z30), (Ra5,Rb2,X2,Z31), (Ra5,Rb2,X2,Z32), (Ra5,Rb2,X2,Z33), (Ra5,Rb2,X2,Z34), (Ra5,Rb2,X2,Z35), (Ra5,Rb2,X2,Z36), (Ra5,Rb2,X2,Z37), (Ra5,Rb2,X2,Z38), (Ra5,Rb2,X2,Z39), (Ra5,Rb3,X1,Z1), (Ra5,Rb3,X1,Z2), (Ra5,Rb3,X1,Z3), (Ra5,Rb3,X1,Z4), (Ra5,Rb3,X1,Z5), (Ra5,Rb3,X1,Z6), (Ra5,Rb3,X1,Z7), (Ra5,Rb3,X1,Z8), (Ra5,Rb3,X1,Z9), (Ra5,Rb3,X1,Z10), (Ra5,Rb3,X1,Z11), (Ra5,Rb3,X1,Z12), (Ra5,Rb3,X1,Z13), (Ra5,Rb3,X1,Z14), (Ra5,Rb3,X1,Z15), (Ra5,Rb3,X1,Z16), (Ra5,Rb3,X1,Z17), (Ra5,Rb3,X1,Z18), (Ra5,Rb3,X1,Z19), (Ra5,Rb3,X1,Z20), (Ra5,Rb3,X1,Z21), (Ra5,Rb3,X1,Z22), (Ra5,Rb3,X1,Z23), (Ra5,Rb3,X1,Z24), (Ra5,Rb3,X1,Z25), (Ra5,Rb3,X1,Z26), (Ra5,Rb3,X1,Z27), (Ra5,Rb3,X1,Z28), (Ra5,Rb3,X1,Z29), (Ra5,Rb3,X1,Z30), (Ra5,Rb3,X1,Z31), (Ra5,Rb3,X1,Z32), (Ra5,Rb3,X1,Z33), (Ra5,Rb3,X1,Z34), (Ra5,Rb3,X1,Z35), (Ra5,Rb3,X1,Z36), (Ra5,Rb3,X1,Z37), (Ra5,Rb3,X1,Z38), (Ra5,Rb3,X1,Z39), (Ra5,Rb3,X2,Z1), (Ra5,Rb3,X2,Z2), (Ra5,Rb3,X2,Z3), (Ra5,Rb3,X2,Z4), (Ra5,Rb3,X2,Z5), (Ra5,Rb3,X2,Z6), (Ra5,Rb3,X2,Z7), (Ra5,Rb3,X2,Z8), (Ra5,Rb3,X2,Z9), (Ra5,Rb3,X2,Z10), (Ra5,Rb3,X2,Z11), (Ra5,Rb3,X2,Z12), (Ra5,Rb3,X2,Z13), (Ra5,Rb3,X2,Z14), (Ra5,Rb3,X2,Z15), (Ra5,Rb3,X2,Z16), (Ra5,Rb3,X2,Z17), (Ra5,Rb3,X2,Z18), (Ra5,Rb3,X2,Z19), (Ra5,Rb3,X2,Z20), (Ra5,Rb3,X2,Z21), (Ra5,Rb3,X2,Z22), (Ra5,Rb3,X2,Z23), (Ra5,Rb3,X2,Z24), (Ra5,Rb3,X2,Z25), (Ra5,Rb3,X2,Z26), (Ra5,Rb3,X2,Z27), (Ra5,Rb3,X2,Z28), (Ra5,Rb3,X2,Z29), (Ra5,Rb3,X2,Z30), (Ra5,Rb3,X2,Z31), (Ra5,Rb3,X2,Z32), (Ra5,Rb3,X2,Z33), (Ra5,Rb3,X2,Z34), (Ra5,Rb3,X2,Z35), (Ra5,Rb3,X2,Z36), (Ra5,Rb3,X2,Z37), (Ra5,Rb3,X2,Z38), (Ra5,Rb3,X2,Z39), (Ra5,Rb4,X1,Z1), (Ra5,Rb4,X1,Z2), (Ra5,Rb4,X1,Z3), (Ra5,Rb4,X1,Z4), (Ra5,Rb4,X1,Z5), (Ra5,Rb4,X1,Z6), (Ra5,Rb4,X1,Z7), (Ra5,Rb4,X1,Z8), (Ra5,Rb4,X1,Z9), (Ra5,Rb4,X1,Z10), (Ra5,Rb4,X1,Z11), (Ra5,Rb4,X1,Z12), (Ra5,Rb4,X1,Z13), (Ra5,Rb4,X1,Z14), (Ra5,Rb4,X1,Z15), (Ra5,Rb4,X1,Z16), (Ra5,Rb4,X1,Z17), (Ra5,Rb4,X1,Z18), (Ra5,Rb4,X1,Z19), (Ra5,Rb4,X1,Z20), (Ra5,Rb4,X1,Z21), (Ra5,Rb4,X1,Z22), (Ra5,Rb4,X1,Z23), (Ra5,Rb4,X1,Z24), (Ra5,Rb4,X1,Z25), (Ra5,Rb4,X1,Z26), (Ra5,Rb4,X1,Z27), (Ra5,Rb4,X1,Z28), (Ra5,Rb4,X1,Z29), (Ra5,Rb4,X1,Z30), (Ra5,Rb4,X1,Z31), (Ra5,Rb4,X1,Z32), (Ra5,Rb4,X1,Z33), (Ra5,Rb4,X1,Z34), (Ra5,Rb4,X1,Z35), (Ra5,Rb4,X1,Z36), (Ra5,Rb4,X1,Z37), (Ra5,Rb4,X1,Z38), (Ra5,Rb4,X1,Z39), (Ra5,Rb4,X2,Z1), (Ra5,Rb4,X2,Z2), (Ra5,Rb4,X2,Z3), (Ra5,Rb4,X2,Z4), (Ra5,Rb4,X2,Z5), (Ra5,Rb4,X2,Z6), (Ra5,Rb4,X2,Z7), (Ra5,Rb4,X2,Z8), (Ra5,Rb4,X2,Z9), (Ra5,Rb4,X2,Z10), (Ra5,Rb4,X2,Z11), (Ra5,Rb4,X2,Z12), (Ra5,Rb4,X2,Z13), (Ra5,Rb4,X2,Z14), (Ra5,Rb4,X2,Z15), (Ra5,Rb4,X2,Z16), (Ra5,Rb4,X2,Z17), (Ra5,Rb4,X2,Z18), (Ra5,Rb4,X2,Z19), (Ra5,Rb4,X2,Z20), (Ra5,Rb4,X2,Z21), (Ra5,Rb4,X2,Z22), (Ra5,Rb4,X2,Z23), (Ra5,Rb4,X2,Z24), (Ra5,Rb4,X2,Z25), (Ra5,Rb4,X2,Z26), (Ra5,Rb4,X2,Z27), (Ra5,Rb4,X2,Z28), (Ra5,Rb4,X2,Z29), (Ra5,Rb4,X2,Z30), (Ra5,Rb4,X2,Z31), (Ra5,Rb4,X2,Z32), (Ra5,Rb4,X2,Z33), (Ra5,Rb4,X2,Z34), (Ra5,Rb4,X2,Z35), (Ra5,Rb4,X2,Z36), (Ra5,Rb4,X2,Z37), (Ra5,Rb4,X2,Z38), (Ra5,Rb4,X2,Z39), (Ra5,Rb5,X1,Z1), (Ra5,Rb5,X1,Z2), (Ra5,Rb5,X1,Z3), (Ra5,Rb5,X1,Z4), (Ra5,Rb5,X1,Z5), (Ra5,Rb5,X1,Z6), (Ra5,Rb5,X1,Z7), (Ra5,Rb5,X1,Z8), (Ra5,Rb5,X1,Z9), (Ra5,Rb5,X1,Z10), (Ra5,Rb5,X1,Z11), (Ra5,Rb5,X1,Z12), (Ra5,Rb5,X1,Z13), (Ra5,Rb5,X1,Z14), (Ra5,Rb5,X1,Z15), (Ra5,Rb5,X1,Z16), (Ra5,Rb5,X1,Z17), (Ra5,Rb5,X1,Z18), (Ra5,Rb5,X1,Z19), (Ra5,Rb5,X1,Z20), (Ra5,Rb5,X1,Z21), (Ra5,Rb5,X1,Z22), (Ra5,Rb5,X1,Z23), (Ra5,Rb5,X1,Z24), (Ra5,Rb5,X1,Z25), (Ra5,Rb5,X1,Z26), (Ra5,Rb5,X1,Z27), (Ra5,Rb5,X1,Z28), (Ra5,Rb5,X1,Z29), (Ra5,Rb5,X1,Z30), (Ra5,Rb5,X1,Z31), (Ra5,Rb5,X1,Z32), (Ra5,Rb5,X1,Z33), (Ra5,Rb5,X1,Z34), (Ra5,Rb5,X1,Z35), (Ra5,Rb5,X1,Z36), (Ra5,Rb5,X1,Z37), (Ra5,Rb5,X1,Z38), (Ra5,Rb5,X1,Z39), (Ra5,Rb5,X2,Z1), (Ra5,Rb5,X2,Z2), (Ra5,Rb5,X2,Z3), (Ra5,Rb5,X2,Z4), (Ra5,Rb5,X2,Z5), (Ra5,Rb5,X2,Z6), (Ra5,Rb5,X2,Z7), (Ra5,Rb5,X2,Z8), (Ra5,Rb5,X2,Z9), (Ra5,Rb5,X2,Z10), (Ra5,Rb5,X2,Z11), (Ra5,Rb5,X2,Z12), (Ra5,Rb5,X2,Z13), (Ra5,Rb5,X2,Z14), (Ra5,Rb5,X2,Z15), (Ra5,Rb5,X2,Z16), (Ra5,Rb5,X2,Z17), (Ra5,Rb5,X2,Z18), (Ra5,Rb5,X2,Z19), (Ra5,Rb5,X2,Z20), (Ra5,Rb5,X2,Z21), (Ra5,Rb5,X2,Z22), (Ra5,Rb5,X2,Z23), (Ra5,Rb5,X2,Z24), (Ra5,Rb5,X2,Z25), (Ra5,Rb5,X2,Z26), (Ra5,Rb5,X2,Z27), (Ra5,Rb5,X2,Z28), (Ra5,Rb5,X2,Z29), (Ra5,Rb5,X2,Z30), (Ra5,Rb5,X2,Z31), (Ra5,Rb5,X2,Z32), (Ra5,Rb5,X2,Z33), (Ra5,Rb5,X2,Z34), (Ra5,Rb5,X2,Z35), (Ra5,Rb5,X2,Z36), (Ra5,Rb5,X2,Z37), (Ra5,Rb5,X2,Z38), (Ra5,Rb5,X2,Z39), (Ra5,Rb6,X1,Z1), (Ra5,Rb6,X1,Z2), (Ra5,Rb6,X1,Z3), (Ra5,Rb6,X1,Z4), (Ra5,Rb6,X1,Z5), (Ra5,Rb6,X1,Z6), (Ra5,Rb6,X1,Z7), (Ra5,Rb6,X1,Z8), (Ra5,Rb6,X1,Z9), (Ra5,Rb6,X1,Z10), (Ra5,Rb6,X1,Z11), (Ra5,Rb6,X1,Z12), (Ra5,Rb6,X1,Z13), (Ra5,Rb6,X1,Z14), (Ra5,Rb6,X1,Z15), (Ra5,Rb6,X1,Z16), (Ra5,Rb6,X1,Z17), (Ra5,Rb6,X1,Z18), (Ra5,Rb6,X1,Z19), (Ra5,Rb6,X1,Z20), (Ra5,Rb6,X1,Z21), (Ra5,Rb6,X1,Z22), (Ra5,Rb6,X1,Z23), (Ra5,Rb6,X1,Z24), (Ra5,Rb6,X1,Z25), (Ra5,Rb6,X1,Z26), (Ra5,Rb6,X1,Z27), (Ra5,Rb6,X1,Z28), (Ra5,Rb6,X1,Z29), (Ra5,Rb6,X1,Z30), (Ra5,Rb6,X1,Z31), (Ra5,Rb6,X1,Z32), (Ra5,Rb6,X1,Z33), (Ra5,Rb6,X1,Z34), (Ra5,Rb6,X1,Z35), (Ra5,Rb6,X1,Z36), (Ra5,Rb6,X1,Z37), (Ra5,Rb6,X1,Z38), (Ra5,Rb6,X1,Z39), (Ra5,Rb6,X2,Z1), (Ra5,Rb6,X2,Z2), (Ra5,Rb6,X2,Z3), (Ra5,Rb6,X2,Z4), (Ra5,Rb6,X2,Z5), (Ra5,Rb6,X2,Z6), (Ra5,Rb6,X2,Z7), (Ra5,Rb6,X2,Z8), (Ra5,Rb6,X2,Z9), (Ra5,Rb6,X2,Z10), (Ra5,Rb6,X2,Z11), (Ra5,Rb6,X2,Z12), (Ra5,Rb6,X2,Z13), (Ra5,Rb6,X2,Z14), (Ra5,Rb6,X2,Z15), (Ra5,Rb6,X2,Z16), (Ra5,Rb6,X2,Z17), (Ra5,Rb6,X2,Z18), (Ra5,Rb6,X2,Z19), (Ra5,Rb6,X2,Z20), (Ra5,Rb6,X2,Z21), (Ra5,Rb6,X2,Z22), (Ra5,Rb6,X2,Z23), (Ra5,Rb6,X2,Z24), (Ra5,Rb6,X2,Z25), (Ra5,Rb6,X2,Z26), (Ra5,Rb6,X2,Z27), (Ra5,Rb6,X2,Z28), (Ra5,Rb6,X2,Z29), (Ra5,Rb6,X2,Z30), (Ra5,Rb6,X2,Z31), (Ra5,Rb6,X2,Z32), (Ra5,Rb6,X2,Z33), (Ra5,Rb6,X2,Z34), (Ra5,Rb6,X2,Z35), (Ra5,Rb6,X2,Z36), (Ra5,Rb6,X2,Z37), (Ra5,Rb6,X2,Z38), (Ra5,Rb6,X2,Z39), (Ra5,Rb7,X1,Z1), (Ra5,Rb7,X1,Z2), (Ra5,Rb7,X1,Z3), 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(Ra5,Rb8,X1,Z38), (Ra5,Rb8,X1,Z39), (Ra5,Rb8,X2,Z1), (Ra5,Rb8,X2,Z2), (Ra5,Rb8,X2,Z3), (Ra5,Rb8,X2,Z4), (Ra5,Rb8,X2,Z5), (Ra5,Rb8,X2,Z6), (Ra5,Rb8,X2,Z7), (Ra5,Rb8,X2,Z8), (Ra5,Rb8,X2,Z9), (Ra5,Rb8,X2,Z10), (Ra5,Rb8,X2,Z11), (Ra5,Rb8,X2,Z12), (Ra5,Rb8,X2,Z13), (Ra5,Rb8,X2,Z14), (Ra5,Rb8,X2,Z15), (Ra5,Rb8,X2,Z16), (Ra5,Rb8,X2,Z17), (Ra5,Rb8,X2,Z18), (Ra5,Rb8,X2,Z19), (Ra5,Rb8,X2,Z20), (Ra5,Rb8,X2,Z21), (Ra5,Rb8,X2,Z22), (Ra5,Rb8,X2,Z23), (Ra5,Rb8,X2,Z24), (Ra5,Rb8,X2,Z25), (Ra5,Rb8,X2,Z26), (Ra5,Rb8,X2,Z27), (Ra5,Rb8,X2,Z28), (Ra5,Rb8,X2,Z29), (Ra5,Rb8,X2,Z30), (Ra5,Rb8,X2,Z31), (Ra5,Rb8,X2,Z32), (Ra5,Rb8,X2,Z33), (Ra5,Rb8,X2,Z34), (Ra5,Rb8,X2,Z35), (Ra5,Rb8,X2,Z36), (Ra5,Rb8,X2,Z37), (Ra5,Rb8,X2,Z38), (Ra5,Rb8,X2,Z39), (Ra6,Rb1,X1,Z1), (Ra6,Rb1,X1,Z2), (Ra6,Rb1,X1,Z3), (Ra6,Rb1,X1,Z4), (Ra6,Rb1,X1,Z5), (Ra6,Rb1,X1,Z6), (Ra6,Rb1,X1,Z7), (Ra6,Rb1,X1,Z8), (Ra6,Rb1,X1,Z9), (Ra6,Rb1,X1,Z10), (Ra6,Rb1,X1,Z11), (Ra6,Rb1,X1,Z12), (Ra6,Rb1,X1,Z13), (Ra6,Rb1,X1,Z14), (Ra6,Rb1,X1,Z15), (Ra6,Rb1,X1,Z16), (Ra6,Rb1,X1,Z17), (Ra6,Rb1,X1,Z18), (Ra6,Rb1,X1,Z19), (Ra6,Rb1,X1,Z20), (Ra6,Rb1,X1,Z21), (Ra6,Rb1,X1,Z22), (Ra6,Rb1,X1,Z23), (Ra6,Rb1,X1,Z24), (Ra6,Rb1,X1,Z25), (Ra6,Rb1,X1,Z26), (Ra6,Rb1,X1,Z27), (Ra6,Rb1,X1,Z28), (Ra6,Rb1,X1,Z29), (Ra6,Rb1,X1,Z30), (Ra6,Rb1,X1,Z31), (Ra6,Rb1,X1,Z32), (Ra6,Rb1,X1,Z33), (Ra6,Rb1,X1,Z34), (Ra6,Rb1,X1,Z35), (Ra6,Rb1,X1,Z36), (Ra6,Rb1,X1,Z37), (Ra6,Rb1,X1,Z38), (Ra6,Rb1,X1,Z39), (Ra6,Rb1,X2,Z1), (Ra6,Rb1,X2,Z2), (Ra6,Rb1,X2,Z3), (Ra6,Rb1,X2,Z4), (Ra6,Rb1,X2,Z5), (Ra6,Rb1,X2,Z6), (Ra6,Rb1,X2,Z7), (Ra6,Rb1,X2,Z8), (Ra6,Rb1,X2,Z9), (Ra6,Rb1,X2,Z10), (Ra6,Rb1,X2,Z11), (Ra6,Rb1,X2,Z12), (Ra6,Rb1,X2,Z13), (Ra6,Rb1,X2,Z14), (Ra6,Rb1,X2,Z15), (Ra6,Rb1,X2,Z16), (Ra6,Rb1,X2,Z17), (Ra6,Rb1,X2,Z18), (Ra6,Rb1,X2,Z19), (Ra6,Rb1,X2,Z20), (Ra6,Rb1,X2,Z21), (Ra6,Rb1,X2,Z22), (Ra6,Rb1,X2,Z23), (Ra6,Rb1,X2,Z24), (Ra6,Rb1,X2,Z25), (Ra6,Rb1,X2,Z26), (Ra6,Rb1,X2,Z27), (Ra6,Rb1,X2,Z28), (Ra6,Rb1,X2,Z29), (Ra6,Rb1,X2,Z30), (Ra6,Rb1,X2,Z31), (Ra6,Rb1,X2,Z32), (Ra6,Rb1,X2,Z33), (Ra6,Rb1,X2,Z34), (Ra6,Rb1,X2,Z35), (Ra6,Rb1,X2,Z36), (Ra6,Rb1,X2,Z37), (Ra6,Rb1,X2,Z38), (Ra6,Rb1,X2,Z39), (Ra6,Rb2,X1,Z1), (Ra6,Rb2,X1,Z2), (Ra6,Rb2,X1,Z3), (Ra6,Rb2,X1,Z4), (Ra6,Rb2,X1,Z5), (Ra6,Rb2,X1,Z6), (Ra6,Rb2,X1,Z7), (Ra6,Rb2,X1,Z8), (Ra6,Rb2,X1,Z9), (Ra6,Rb2,X1,Z10), (Ra6,Rb2,X1,Z11), (Ra6,Rb2,X1,Z12), (Ra6,Rb2,X1,Z13), (Ra6,Rb2,X1,Z14), (Ra6,Rb2,X1,Z15), (Ra6,Rb2,X1,Z16), (Ra6,Rb2,X1,Z17), (Ra6,Rb2,X1,Z18), (Ra6,Rb2,X1,Z19), (Ra6,Rb2,X1,Z20), (Ra6,Rb2,X1,Z21), (Ra6,Rb2,X1,Z22), (Ra6,Rb2,X1,Z23), (Ra6,Rb2,X1,Z24), (Ra6,Rb2,X1,Z25), (Ra6,Rb2,X1,Z26), (Ra6,Rb2,X1,Z27), (Ra6,Rb2,X1,Z28), (Ra6,Rb2,X1,Z29), (Ra6,Rb2,X1,Z30), (Ra6,Rb2,X1,Z31), (Ra6,Rb2,X1,Z32), (Ra6,Rb2,X1,Z33), (Ra6,Rb2,X1,Z34), (Ra6,Rb2,X1,Z35), (Ra6,Rb2,X1,Z36), (Ra6,Rb2,X1,Z37), (Ra6,Rb2,X1,Z38), (Ra6,Rb2,X1,Z39), (Ra6,Rb2,X2,Z1), (Ra6,Rb2,X2,Z2), (Ra6,Rb2,X2,Z3), (Ra6,Rb2,X2,Z4), (Ra6,Rb2,X2,Z5), (Ra6,Rb2,X2,Z6), (Ra6,Rb2,X2,Z7), (Ra6,Rb2,X2,Z8), (Ra6,Rb2,X2,Z9), (Ra6,Rb2,X2,Z10), 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(Ra6,Rb3,X1,Z28), (Ra6,Rb3,X1,Z29), (Ra6,Rb3,X1,Z30), (Ra6,Rb3,X1,Z31), (Ra6,Rb3,X1,Z32), (Ra6,Rb3,X1,Z33), (Ra6,Rb3,X1,Z34), (Ra6,Rb3,X1,Z35), (Ra6,Rb3,X1,Z36), (Ra6,Rb3,X1,Z37), (Ra6,Rb3,X1,Z38), (Ra6,Rb3,X1,Z39), (Ra6,Rb3,X2,Z1), (Ra6,Rb3,X2,Z2), (Ra6,Rb3,X2,Z3), (Ra6,Rb3,X2,Z4), (Ra6,Rb3,X2,Z5), (Ra6,Rb3,X2,Z6), (Ra6,Rb3,X2,Z7), (Ra6,Rb3,X2,Z8), (Ra6,Rb3,X2,Z9), (Ra6,Rb3,X2,Z10), (Ra6,Rb3,X2,Z11), (Ra6,Rb3,X2,Z12), (Ra6,Rb3,X2,Z13), (Ra6,Rb3,X2,Z14), (Ra6,Rb3,X2,Z15), (Ra6,Rb3,X2,Z16), (Ra6,Rb3,X2,Z17), (Ra6,Rb3,X2,Z18), (Ra6,Rb3,X2,Z19), (Ra6,Rb3,X2,Z20), (Ra6,Rb3,X2,Z21), (Ra6,Rb3,X2,Z22), (Ra6,Rb3,X2,Z23), (Ra6,Rb3,X2,Z24), (Ra6,Rb3,X2,Z25), (Ra6,Rb3,X2,Z26), (Ra6,Rb3,X2,Z27), (Ra6,Rb3,X2,Z28), (Ra6,Rb3,X2,Z29), (Ra6,Rb3,X2,Z30), (Ra6,Rb3,X2,Z31), (Ra6,Rb3,X2,Z32), (Ra6,Rb3,X2,Z33), (Ra6,Rb3,X2,Z34), (Ra6,Rb3,X2,Z35), (Ra6,Rb3,X2,Z36), (Ra6,Rb3,X2,Z37), (Ra6,Rb3,X2,Z38), (Ra6,Rb3,X2,Z39), (Ra6,Rb4,X1,Z1), (Ra6,Rb4,X1,Z2), (Ra6,Rb4,X1,Z3), (Ra6,Rb4,X1,Z4), (Ra6,Rb4,X1,Z5), (Ra6,Rb4,X1,Z6), (Ra6,Rb4,X1,Z7), (Ra6,Rb4,X1,Z8), (Ra6,Rb4,X1,Z9), (Ra6,Rb4,X1,Z10), (Ra6,Rb4,X1,Z11), (Ra6,Rb4,X1,Z12), (Ra6,Rb4,X1,Z13), (Ra6,Rb4,X1,Z14), (Ra6,Rb4,X1,Z15), (Ra6,Rb4,X1,Z16), (Ra6,Rb4,X1,Z17), (Ra6,Rb4,X1,Z18), (Ra6,Rb4,X1,Z19), (Ra6,Rb4,X1,Z20), (Ra6,Rb4,X1,Z21), (Ra6,Rb4,X1,Z22), (Ra6,Rb4,X1,Z23), (Ra6,Rb4,X1,Z24), (Ra6,Rb4,X1,Z25), (Ra6,Rb4,X1,Z26), (Ra6,Rb4,X1,Z27), (Ra6,Rb4,X1,Z28), (Ra6,Rb4,X1,Z29), (Ra6,Rb4,X1,Z30), (Ra6,Rb4,X1,Z31), (Ra6,Rb4,X1,Z32), (Ra6,Rb4,X1,Z33), (Ra6,Rb4,X1,Z34), (Ra6,Rb4,X1,Z35), (Ra6,Rb4,X1,Z36), (Ra6,Rb4,X1,Z37), (Ra6,Rb4,X1,Z38), (Ra6,Rb4,X1,Z39), (Ra6,Rb4,X2,Z1), (Ra6,Rb4,X2,Z2), (Ra6,Rb4,X2,Z3), (Ra6,Rb4,X2,Z4), (Ra6,Rb4,X2,Z5), (Ra6,Rb4,X2,Z6), (Ra6,Rb4,X2,Z7), (Ra6,Rb4,X2,Z8), (Ra6,Rb4,X2,Z9), (Ra6,Rb4,X2,Z10), (Ra6,Rb4,X2,Z11), (Ra6,Rb4,X2,Z12), (Ra6,Rb4,X2,Z13), (Ra6,Rb4,X2,Z14), (Ra6,Rb4,X2,Z15), (Ra6,Rb4,X2,Z16), (Ra6,Rb4,X2,Z17), (Ra6,Rb4,X2,Z18), (Ra6,Rb4,X2,Z19), (Ra6,Rb4,X2,Z20), (Ra6,Rb4,X2,Z21), (Ra6,Rb4,X2,Z22), 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(Ra6,Rb6,X2,Z35), (Ra6,Rb6,X2,Z36), (Ra6,Rb6,X2,Z37), (Ra6,Rb6,X2,Z38), (Ra6,Rb6,X2,Z39), (Ra6,Rb7,X1,Z1), (Ra6,Rb7,X1,Z2), (Ra6,Rb7,X1,Z3), (Ra6,Rb7,X1,Z4), (Ra6,Rb7,X1,Z5), (Ra6,Rb7,X1,Z6), (Ra6,Rb7,X1,Z7), (Ra6,Rb7,X1,Z8), (Ra6,Rb7,X1,Z9), (Ra6,Rb7,X1,Z10), (Ra6,Rb7,X1,Z11), (Ra6,Rb7,X1,Z12), (Ra6,Rb7,X1,Z13), (Ra6,Rb7,X1,Z14), (Ra6,Rb7,X1,Z15), (Ra6,Rb7,X1,Z16), (Ra6,Rb7,X1,Z17), (Ra6,Rb7,X1,Z18), (Ra6,Rb7,X1,Z19), (Ra6,Rb7,X1,Z20), (Ra6,Rb7,X1,Z21), (Ra6,Rb7,X1,Z22), (Ra6,Rb7,X1,Z23), (Ra6,Rb7,X1,Z24), (Ra6,Rb7,X1,Z25), (Ra6,Rb7,X1,Z26), (Ra6,Rb7,X1,Z27), (Ra6,Rb7,X1,Z28), (Ra6,Rb7,X1,Z29), (Ra6,Rb7,X1,Z30), (Ra6,Rb7,X1,Z31), (Ra6,Rb7,X1,Z32), (Ra6,Rb7,X1,Z33), (Ra6,Rb7,X1,Z34), (Ra6,Rb7,X1,Z35), (Ra6,Rb7,X1,Z36), (Ra6,Rb7,X1,Z37), (Ra6,Rb7,X1,Z38), (Ra6,Rb7,X1,Z39), (Ra6,Rb7,X2,Z1), (Ra6,Rb7,X2,Z2), (Ra6,Rb7,X2,Z3), (Ra6,Rb7,X2,Z4), (Ra6,Rb7,X2,Z5), (Ra6,Rb7,X2,Z6), (Ra6,Rb7,X2,Z7), (Ra6,Rb7,X2,Z8), (Ra6,Rb7,X2,Z9), (Ra6,Rb7,X2,Z10), (Ra6,Rb7,X2,Z11), (Ra6,Rb7,X2,Z12), (Ra6,Rb7,X2,Z13), (Ra6,Rb7,X2,Z14), (Ra6,Rb7,X2,Z15), (Ra6,Rb7,X2,Z16), (Ra6,Rb7,X2,Z17), (Ra6,Rb7,X2,Z18), (Ra6,Rb7,X2,Z19), (Ra6,Rb7,X2,Z20), (Ra6,Rb7,X2,Z21), (Ra6,Rb7,X2,Z22), (Ra6,Rb7,X2,Z23), (Ra6,Rb7,X2,Z24), (Ra6,Rb7,X2,Z25), (Ra6,Rb7,X2,Z26), (Ra6,Rb7,X2,Z27), (Ra6,Rb7,X2,Z28), (Ra6,Rb7,X2,Z29), (Ra6,Rb7,X2,Z30), (Ra6,Rb7,X2,Z31), (Ra6,Rb7,X2,Z32), (Ra6,Rb7,X2,Z33), (Ra6,Rb7,X2,Z34), (Ra6,Rb7,X2,Z35), (Ra6,Rb7,X2,Z36), (Ra6,Rb7,X2,Z37), (Ra6,Rb7,X2,Z38), (Ra6,Rb7,X2,Z39), (Ra6,Rb8,X1,Z1), (Ra6,Rb8,X1,Z2), (Ra6,Rb8,X1,Z3), (Ra6,Rb8,X1,Z4), (Ra6,Rb8,X1,Z5), (Ra6,Rb8,X1,Z6), (Ra6,Rb8,X1,Z7), (Ra6,Rb8,X1,Z8), (Ra6,Rb8,X1,Z9), (Ra6,Rb8,X1,Z10), (Ra6,Rb8,X1,Z11), (Ra6,Rb8,X1,Z12), (Ra6,Rb8,X1,Z13), (Ra6,Rb8,X1,Z14), (Ra6,Rb8,X1,Z15), (Ra6,Rb8,X1,Z16), (Ra6,Rb8,X1,Z17), (Ra6,Rb8,X1,Z18), (Ra6,Rb8,X1,Z19), (Ra6,Rb8,X1,Z20), (Ra6,Rb8,X1,Z21), (Ra6,Rb8,X1,Z22), (Ra6,Rb8,X1,Z23), (Ra6,Rb8,X1,Z24), (Ra6,Rb8,X1,Z25), (Ra6,Rb8,X1,Z26), (Ra6,Rb8,X1,Z27), (Ra6,Rb8,X1,Z28), (Ra6,Rb8,X1,Z29), (Ra6,Rb8,X1,Z30), (Ra6,Rb8,X1,Z31), (Ra6,Rb8,X1,Z32), (Ra6,Rb8,X1,Z33), (Ra6,Rb8,X1,Z34), (Ra6,Rb8,X1,Z35), (Ra6,Rb8,X1,Z36), (Ra6,Rb8,X1,Z37), (Ra6,Rb8,X1,Z38), (Ra6,Rb8,X1,Z39), (Ra6,Rb8,X2,Z1), (Ra6,Rb8,X2,Z2), (Ra6,Rb8,X2,Z3), (Ra6,Rb8,X2,Z4), (Ra6,Rb8,X2,Z5), (Ra6,Rb8,X2,Z6), (Ra6,Rb8,X2,Z7), (Ra6,Rb8,X2,Z8), (Ra6,Rb8,X2,Z9), (Ra6,Rb8,X2,Z10), (Ra6,Rb8,X2,Z11), (Ra6,Rb8,X2,Z12), (Ra6,Rb8,X2,Z13), (Ra6,Rb8,X2,Z14), (Ra6,Rb8,X2,Z15), (Ra6,Rb8,X2,Z16), (Ra6,Rb8,X2,Z17), (Ra6,Rb8,X2,Z18), (Ra6,Rb8,X2,Z19), (Ra6,Rb8,X2,Z20), (Ra6,Rb8,X2,Z21), (Ra6,Rb8,X2,Z22), (Ra6,Rb8,X2,Z23), (Ra6,Rb8,X2,Z24), (Ra6,Rb8,X2,Z25), (Ra6,Rb8,X2,Z26), (Ra6,Rb8,X2,Z27), (Ra6,Rb8,X2,Z28), (Ra6,Rb8,X2,Z29), (Ra6,Rb8,X2,Z30), (Ra6,Rb8,X2,Z31), (Ra6,Rb8,X2,Z32), (Ra6,Rb8,X2,Z33), (Ra6,Rb8,X2,Z34), (Ra6,Rb8,X2,Z35), (Ra6,Rb8,X2,Z36), (Ra6,Rb8,X2,Z37), (Ra6,Rb8,X2,Z38), (Ra6,Rb8,X2,Z39), (Ra7,Rb1,X1,Z1), (Ra7,Rb1,X1,Z2), (Ra7,Rb1,X1,Z3), (Ra7,Rb1,X1,Z4), (Ra7,Rb1,X1,Z5), (Ra7,Rb1,X1,Z6), (Ra7,Rb1,X1,Z7), (Ra7,Rb1,X1,Z8), (Ra7,Rb1,X1,Z9), (Ra7,Rb1,X1,Z10), (Ra7,Rb1,X1,Z11), (Ra7,Rb1,X1,Z12), (Ra7,Rb1,X1,Z13), (Ra7,Rb1,X1,Z14), (Ra7,Rb1,X1,Z15), (Ra7,Rb1,X1,Z16), (Ra7,Rb1,X1,Z17), (Ra7,Rb1,X1,Z18), (Ra7,Rb1,X1,Z19), (Ra7,Rb1,X1,Z20), (Ra7,Rb1,X1,Z21), (Ra7,Rb1,X1,Z22), (Ra7,Rb1,X1,Z23), (Ra7,Rb1,X1,Z24), (Ra7,Rb1,X1,Z25), (Ra7,Rb1,X1,Z26), (Ra7,Rb1,X1,Z27), (Ra7,Rb1,X1,Z28), (Ra7,Rb1,X1,Z29), (Ra7,Rb1,X1,Z30), (Ra7,Rb1,X1,Z31), (Ra7,Rb1,X1,Z32), (Ra7,Rb1,X1,Z33), (Ra7,Rb1,X1,Z34), (Ra7,Rb1,X1,Z35), (Ra7,Rb1,X1,Z36), (Ra7,Rb1,X1,Z37), (Ra7,Rb1,X1,Z38), (Ra7,Rb1,X1,Z39), (Ra7,Rb1,X2,Z1), (Ra7,Rb1,X2,Z2), (Ra7,Rb1,X2,Z3), (Ra7,Rb1,X2,Z4), (Ra7,Rb1,X2,Z5), (Ra7,Rb1,X2,Z6), (Ra7,Rb1,X2,Z7), (Ra7,Rb1,X2,Z8), (Ra7,Rb1,X2,Z9), (Ra7,Rb1,X2,Z10), (Ra7,Rb1,X2,Z11), (Ra7,Rb1,X2,Z12), (Ra7,Rb1,X2,Z13), (Ra7,Rb1,X2,Z14), (Ra7,Rb1,X2,Z15), (Ra7,Rb1,X2,Z16), (Ra7,Rb1,X2,Z17), (Ra7,Rb1,X2,Z18), (Ra7,Rb1,X2,Z19), (Ra7,Rb1,X2,Z20), (Ra7,Rb1,X2,Z21), (Ra7,Rb1,X2,Z22), (Ra7,Rb1,X2,Z23), (Ra7,Rb1,X2,Z24), (Ra7,Rb1,X2,Z25), (Ra7,Rb1,X2,Z26), (Ra7,Rb1,X2,Z27), (Ra7,Rb1,X2,Z28), (Ra7,Rb1,X2,Z29), (Ra7,Rb1,X2,Z30), (Ra7,Rb1,X2,Z31), (Ra7,Rb1,X2,Z32), (Ra7,Rb1,X2,Z33), (Ra7,Rb1,X2,Z34), (Ra7,Rb1,X2,Z35), (Ra7,Rb1,X2,Z36), (Ra7,Rb1,X2,Z37), (Ra7,Rb1,X2,Z38), (Ra7,Rb1,X2,Z39), (Ra7,Rb2,X1,Z1), (Ra7,Rb2,X1,Z2), (Ra7,Rb2,X1,Z3), (Ra7,Rb2,X1,Z4), (Ra7,Rb2,X1,Z5), (Ra7,Rb2,X1,Z6), (Ra7,Rb2,X1,Z7), (Ra7,Rb2,X1,Z8), (Ra7,Rb2,X1,Z9), (Ra7,Rb2,X1,Z10), (Ra7,Rb2,X1,Z11), (Ra7,Rb2,X1,Z12), (Ra7,Rb2,X1,Z13), (Ra7,Rb2,X1,Z14), (Ra7,Rb2,X1,Z15), (Ra7,Rb2,X1,Z16), (Ra7,Rb2,X1,Z17), (Ra7,Rb2,X1,Z18), (Ra7,Rb2,X1,Z19), (Ra7,Rb2,X1,Z20), (Ra7,Rb2,X1,Z21), (Ra7,Rb2,X1,Z22), (Ra7,Rb2,X1,Z23), (Ra7,Rb2,X1,Z24), (Ra7,Rb2,X1,Z25), (Ra7,Rb2,X1,Z26), (Ra7,Rb2,X1,Z27), (Ra7,Rb2,X1,Z28), (Ra7,Rb2,X1,Z29), (Ra7,Rb2,X1,Z30), (Ra7,Rb2,X1,Z31), (Ra7,Rb2,X1,Z32), (Ra7,Rb2,X1,Z33), (Ra7,Rb2,X1,Z34), (Ra7,Rb2,X1,Z35), (Ra7,Rb2,X1,Z36), (Ra7,Rb2,X1,Z37), (Ra7,Rb2,X1,Z38), (Ra7,Rb2,X1,Z39), (Ra7,Rb2,X2,Z1), (Ra7,Rb2,X2,Z2), (Ra7,Rb2,X2,Z3), (Ra7,Rb2,X2,Z4), (Ra7,Rb2,X2,Z5), (Ra7,Rb2,X2,Z6), (Ra7,Rb2,X2,Z7), (Ra7,Rb2,X2,Z8), (Ra7,Rb2,X2,Z9), (Ra7,Rb2,X2,Z10), (Ra7,Rb2,X2,Z11), (Ra7,Rb2,X2,Z12), (Ra7,Rb2,X2,Z13), (Ra7,Rb2,X2,Z14), (Ra7,Rb2,X2,Z15), (Ra7,Rb2,X2,Z16), (Ra7,Rb2,X2,Z17), (Ra7,Rb2,X2,Z18), (Ra7,Rb2,X2,Z19), (Ra7,Rb2,X2,Z20), (Ra7,Rb2,X2,Z21), (Ra7,Rb2,X2,Z22), (Ra7,Rb2,X2,Z23), (Ra7,Rb2,X2,Z24), (Ra7,Rb2,X2,Z25), (Ra7,Rb2,X2,Z26), (Ra7,Rb2,X2,Z27), (Ra7,Rb2,X2,Z28), (Ra7,Rb2,X2,Z29), (Ra7,Rb2,X2,Z30), (Ra7,Rb2,X2,Z31), (Ra7,Rb2,X2,Z32), (Ra7,Rb2,X2,Z33), (Ra7,Rb2,X2,Z34), (Ra7,Rb2,X2,Z35), (Ra7,Rb2,X2,Z36), (Ra7,Rb2,X2,Z37), (Ra7,Rb2,X2,Z38), (Ra7,Rb2,X2,Z39), (Ra7,Rb3,X1,Z1), (Ra7,Rb3,X1,Z2), (Ra7,Rb3,X1,Z3), (Ra7,Rb3,X1,Z4), (Ra7,Rb3,X1,Z5), (Ra7,Rb3,X1,Z6), (Ra7,Rb3,X1,Z7), (Ra7,Rb3,X1,Z8), (Ra7,Rb3,X1,Z9), (Ra7,Rb3,X1,Z10), (Ra7,Rb3,X1,Z11), (Ra7,Rb3,X1,Z12), (Ra7,Rb3,X1,Z13), (Ra7,Rb3,X1,Z14), (Ra7,Rb3,X1,Z15), (Ra7,Rb3,X1,Z16), (Ra7,Rb3,X1,Z17), (Ra7,Rb3,X1,Z18), (Ra7,Rb3,X1,Z19), (Ra7,Rb3,X1,Z20), (Ra7,Rb3,X1,Z21), (Ra7,Rb3,X1,Z22), (Ra7,Rb3,X1,Z23), (Ra7,Rb3,X1,Z24), (Ra7,Rb3,X1,Z25), (Ra7,Rb3,X1,Z26), (Ra7,Rb3,X1,Z27), (Ra7,Rb3,X1,Z28), (Ra7,Rb3,X1,Z29), (Ra7,Rb3,X1,Z30), (Ra7,Rb3,X1,Z31), (Ra7,Rb3,X1,Z32), (Ra7,Rb3,X1,Z33), (Ra7,Rb3,X1,Z34), (Ra7,Rb3,X1,Z35), (Ra7,Rb3,X1,Z36), (Ra7,Rb3,X1,Z37), (Ra7,Rb3,X1,Z38), (Ra7,Rb3,X1,Z39), (Ra7,Rb3,X2,Z1), (Ra7,Rb3,X2,Z2), (Ra7,Rb3,X2,Z3), (Ra7,Rb3,X2,Z4), (Ra7,Rb3,X2,Z5), (Ra7,Rb3,X2,Z6), (Ra7,Rb3,X2,Z7), (Ra7,Rb3,X2,Z8), (Ra7,Rb3,X2,Z9), (Ra7,Rb3,X2,Z10), (Ra7,Rb3,X2,Z11), (Ra7,Rb3,X2,Z12), (Ra7,Rb3,X2,Z13), (Ra7,Rb3,X2,Z14), (Ra7,Rb3,X2,Z15), (Ra7,Rb3,X2,Z16), (Ra7,Rb3,X2,Z17), (Ra7,Rb3,X2,Z18), (Ra7,Rb3,X2,Z19), (Ra7,Rb3,X2,Z20), (Ra7,Rb3,X2,Z21), (Ra7,Rb3,X2,Z22), (Ra7,Rb3,X2,Z23), (Ra7,Rb3,X2,Z24), (Ra7,Rb3,X2,Z25), (Ra7,Rb3,X2,Z26), (Ra7,Rb3,X2,Z27), (Ra7,Rb3,X2,Z28), (Ra7,Rb3,X2,Z29), (Ra7,Rb3,X2,Z30), (Ra7,Rb3,X2,Z31), (Ra7,Rb3,X2,Z32), (Ra7,Rb3,X2,Z33), (Ra7,Rb3,X2,Z34), (Ra7,Rb3,X2,Z35), (Ra7,Rb3,X2,Z36), (Ra7,Rb3,X2,Z37), (Ra7,Rb3,X2,Z38), (Ra7,Rb3,X2,Z39), (Ra7,Rb4,X1,Z1), (Ra7,Rb4,X1,Z2), (Ra7,Rb4,X1,Z3), (Ra7,Rb4,X1,Z4), (Ra7,Rb4,X1,Z5), (Ra7,Rb4,X1,Z6), (Ra7,Rb4,X1,Z7), (Ra7,Rb4,X1,Z8), (Ra7,Rb4,X1,Z9), (Ra7,Rb4,X1,Z10), (Ra7,Rb4,X1,Z11), (Ra7,Rb4,X1,Z12), (Ra7,Rb4,X1,Z13), (Ra7,Rb4,X1,Z14), (Ra7,Rb4,X1,Z15), (Ra7,Rb4,X1,Z16), (Ra7,Rb4,X1,Z17), (Ra7,Rb4,X1,Z18), (Ra7,Rb4,X1,Z19), (Ra7,Rb4,X1,Z20), (Ra7,Rb4,X1,Z21), (Ra7,Rb4,X1,Z22), (Ra7,Rb4,X1,Z23), (Ra7,Rb4,X1,Z24), (Ra7,Rb4,X1,Z25), (Ra7,Rb4,X1,Z26), (Ra7,Rb4,X1,Z27), (Ra7,Rb4,X1,Z28), (Ra7,Rb4,X1,Z29), (Ra7,Rb4,X1,Z30), (Ra7,Rb4,X1,Z31), (Ra7,Rb4,X1,Z32), (Ra7,Rb4,X1,Z33), (Ra7,Rb4,X1,Z34), (Ra7,Rb4,X1,Z35), (Ra7,Rb4,X1,Z36), (Ra7,Rb4,X1,Z37), (Ra7,Rb4,X1,Z38), (Ra7,Rb4,X1,Z39), (Ra7,Rb4,X2,Z1), (Ra7,Rb4,X2,Z2), (Ra7,Rb4,X2,Z3), (Ra7,Rb4,X2,Z4), (Ra7,Rb4,X2,Z5), (Ra7,Rb4,X2,Z6), (Ra7,Rb4,X2,Z7), (Ra7,Rb4,X2,Z8), (Ra7,Rb4,X2,Z9), (Ra7,Rb4,X2,Z10), (Ra7,Rb4,X2,Z11), (Ra7,Rb4,X2,Z12), (Ra7,Rb4,X2,Z13), (Ra7,Rb4,X2,Z14), (Ra7,Rb4,X2,Z15), (Ra7,Rb4,X2,Z16), (Ra7,Rb4,X2,Z17), (Ra7,Rb4,X2,Z18), (Ra7,Rb4,X2,Z19), (Ra7,Rb4,X2,Z20), (Ra7,Rb4,X2,Z21), (Ra7,Rb4,X2,Z22), (Ra7,Rb4,X2,Z23), (Ra7,Rb4,X2,Z24), (Ra7,Rb4,X2,Z25), (Ra7,Rb4,X2,Z26), (Ra7,Rb4,X2,Z27), (Ra7,Rb4,X2,Z28), (Ra7,Rb4,X2,Z29), (Ra7,Rb4,X2,Z30), (Ra7,Rb4,X2,Z31), (Ra7,Rb4,X2,Z32), (Ra7,Rb4,X2,Z33), (Ra7,Rb4,X2,Z34), (Ra7,Rb4,X2,Z35), (Ra7,Rb4,X2,Z36), (Ra7,Rb4,X2,Z37), (Ra7,Rb4,X2,Z38), (Ra7,Rb4,X2,Z39), (Ra7,Rb5,X1,Z1), (Ra7,Rb5,X1,Z2), (Ra7,Rb5,X1,Z3), (Ra7,Rb5,X1,Z4), (Ra7,Rb5,X1,Z5), (Ra7,Rb5,X1,Z6), (Ra7,Rb5,X1,Z7), (Ra7,Rb5,X1,Z8), (Ra7,Rb5,X1,Z9), (Ra7,Rb5,X1,Z10), (Ra7,Rb5,X1,Z11), (Ra7,Rb5,X1,Z12), (Ra7,Rb5,X1,Z13), (Ra7,Rb5,X1,Z14), (Ra7,Rb5,X1,Z15), (Ra7,Rb5,X1,Z16), (Ra7,Rb5,X1,Z17), (Ra7,Rb5,X1,Z18), (Ra7,Rb5,X1,Z19), (Ra7,Rb5,X1,Z20), (Ra7,Rb5,X1,Z21), (Ra7,Rb5,X1,Z22), (Ra7,Rb5,X1,Z23), (Ra7,Rb5,X1,Z24), (Ra7,Rb5,X1,Z25), (Ra7,Rb5,X1,Z26), (Ra7,Rb5,X1,Z27), (Ra7,Rb5,X1,Z28), (Ra7,Rb5,X1,Z29), (Ra7,Rb5,X1,Z30), (Ra7,Rb5,X1,Z31), (Ra7,Rb5,X1,Z32), (Ra7,Rb5,X1,Z33), (Ra7,Rb5,X1,Z34), (Ra7,Rb5,X1,Z35), (Ra7,Rb5,X1,Z36), (Ra7,Rb5,X1,Z37), (Ra7,Rb5,X1,Z38), (Ra7,Rb5,X1,Z39), (Ra7,Rb5,X2,Z1), (Ra7,Rb5,X2,Z2), (Ra7,Rb5,X2,Z3), (Ra7,Rb5,X2,Z4), (Ra7,Rb5,X2,Z5), (Ra7,Rb5,X2,Z6), (Ra7,Rb5,X2,Z7), (Ra7,Rb5,X2,Z8), (Ra7,Rb5,X2,Z9), (Ra7,Rb5,X2,Z10), (Ra7,Rb5,X2,Z11), (Ra7,Rb5,X2,Z12), (Ra7,Rb5,X2,Z13), (Ra7,Rb5,X2,Z14), (Ra7,Rb5,X2,Z15), (Ra7,Rb5,X2,Z16), (Ra7,Rb5,X2,Z17), (Ra7,Rb5,X2,Z18), (Ra7,Rb5,X2,Z19), (Ra7,Rb5,X2,Z20), (Ra7,Rb5,X2,Z21), (Ra7,Rb5,X2,Z22), (Ra7,Rb5,X2,Z23), (Ra7,Rb5,X2,Z24), (Ra7,Rb5,X2,Z25), (Ra7,Rb5,X2,Z26), (Ra7,Rb5,X2,Z27), (Ra7,Rb5,X2,Z28), (Ra7,Rb5,X2,Z29), (Ra7,Rb5,X2,Z30), (Ra7,Rb5,X2,Z31), (Ra7,Rb5,X2,Z32), (Ra7,Rb5,X2,Z33), (Ra7,Rb5,X2,Z34), (Ra7,Rb5,X2,Z35), (Ra7,Rb5,X2,Z36), (Ra7,Rb5,X2,Z37), (Ra7,Rb5,X2,Z38), (Ra7,Rb5,X2,Z39), (Ra7,Rb6,X1,Z1), (Ra7,Rb6,X1,Z2), (Ra7,Rb6,X1,Z3), (Ra7,Rb6,X1,Z4), (Ra7,Rb6,X1,Z5), (Ra7,Rb6,X1,Z6), (Ra7,Rb6,X1,Z7), (Ra7,Rb6,X1,Z8), (Ra7,Rb6,X1,Z9), (Ra7,Rb6,X1,Z10), (Ra7,Rb6,X1,Z11), (Ra7,Rb6,X1,Z12), (Ra7,Rb6,X1,Z13), (Ra7,Rb6,X1,Z14), (Ra7,Rb6,X1,Z15), (Ra7,Rb6,X1,Z16), (Ra7,Rb6,X1,Z17), (Ra7,Rb6,X1,Z18), (Ra7,Rb6,X1,Z19), (Ra7,Rb6,X1,Z20), (Ra7,Rb6,X1,Z21), (Ra7,Rb6,X1,Z22), (Ra7,Rb6,X1,Z23), (Ra7,Rb6,X1,Z24), (Ra7,Rb6,X1,Z25), (Ra7,Rb6,X1,Z26), (Ra7,Rb6,X1,Z27), (Ra7,Rb6,X1,Z28), (Ra7,Rb6,X1,Z29), (Ra7,Rb6,X1,Z30), (Ra7,Rb6,X1,Z31), (Ra7,Rb6,X1,Z32), (Ra7,Rb6,X1,Z33), (Ra7,Rb6,X1,Z34), (Ra7,Rb6,X1,Z35), (Ra7,Rb6,X1,Z36), (Ra7,Rb6,X1,Z37), (Ra7,Rb6,X1,Z38), (Ra7,Rb6,X1,Z39), (Ra7,Rb6,X2,Z1), (Ra7,Rb6,X2,Z2), (Ra7,Rb6,X2,Z3), (Ra7,Rb6,X2,Z4), (Ra7,Rb6,X2,Z5), (Ra7,Rb6,X2,Z6), (Ra7,Rb6,X2,Z7), (Ra7,Rb6,X2,Z8), (Ra7,Rb6,X2,Z9), (Ra7,Rb6,X2,Z10), (Ra7,Rb6,X2,Z11), (Ra7,Rb6,X2,Z12), (Ra7,Rb6,X2,Z13), (Ra7,Rb6,X2,Z14), (Ra7,Rb6,X2,Z15), (Ra7,Rb6,X2,Z16), (Ra7,Rb6,X2,Z17), (Ra7,Rb6,X2,Z18), (Ra7,Rb6,X2,Z19), (Ra7,Rb6,X2,Z20), (Ra7,Rb6,X2,Z21), (Ra7,Rb6,X2,Z22), (Ra7,Rb6,X2,Z23), (Ra7,Rb6,X2,Z24), (Ra7,Rb6,X2,Z25), (Ra7,Rb6,X2,Z26), (Ra7,Rb6,X2,Z27), (Ra7,Rb6,X2,Z28), (Ra7,Rb6,X2,Z29), (Ra7,Rb6,X2,Z30), (Ra7,Rb6,X2,Z31), (Ra7,Rb6,X2,Z32), (Ra7,Rb6,X2,Z33), (Ra7,Rb6,X2,Z34), (Ra7,Rb6,X2,Z35), (Ra7,Rb6,X2,Z36), (Ra7,Rb6,X2,Z37), (Ra7,Rb6,X2,Z38), (Ra7,Rb6,X2,Z39), (Ra7,Rb7,X1,Z1), (Ra7,Rb7,X1,Z2), (Ra7,Rb7,X1,Z3), (Ra7,Rb7,X1,Z4), (Ra7,Rb7,X1,Z5), (Ra7,Rb7,X1,Z6), (Ra7,Rb7,X1,Z7), (Ra7,Rb7,X1,Z8), (Ra7,Rb7,X1,Z9), (Ra7,Rb7,X1,Z10), (Ra7,Rb7,X1,Z11), (Ra7,Rb7,X1,Z12), (Ra7,Rb7,X1,Z13), (Ra7,Rb7,X1,Z14), (Ra7,Rb7,X1,Z15), (Ra7,Rb7,X1,Z16), (Ra7,Rb7,X1,Z17), (Ra7,Rb7,X1,Z18), (Ra7,Rb7,X1,Z19), (Ra7,Rb7,X1,Z20), (Ra7,Rb7,X1,Z21), (Ra7,Rb7,X1,Z22), (Ra7,Rb7,X1,Z23), (Ra7,Rb7,X1,Z24), (Ra7,Rb7,X1,Z25), (Ra7,Rb7,X1,Z26), (Ra7,Rb7,X1,Z27), (Ra7,Rb7,X1,Z28), (Ra7,Rb7,X1,Z29), (Ra7,Rb7,X1,Z30), (Ra7,Rb7,X1,Z31), (Ra7,Rb7,X1,Z32), (Ra7,Rb7,X1,Z33), (Ra7,Rb7,X1,Z34), (Ra7,Rb7,X1,Z35), (Ra7,Rb7,X1,Z36), (Ra7,Rb7,X1,Z37), (Ra7,Rb7,X1,Z38), (Ra7,Rb7,X1,Z39), (Ra7,Rb7,X2,Z1), (Ra7,Rb7,X2,Z2), (Ra7,Rb7,X2,Z3), (Ra7,Rb7,X2,Z4), (Ra7,Rb7,X2,Z5), (Ra7,Rb7,X2,Z6), (Ra7,Rb7,X2,Z7), (Ra7,Rb7,X2,Z8), (Ra7,Rb7,X2,Z9), (Ra7,Rb7,X2,Z10), (Ra7,Rb7,X2,Z11), (Ra7,Rb7,X2,Z12), (Ra7,Rb7,X2,Z13), (Ra7,Rb7,X2,Z14), (Ra7,Rb7,X2,Z15), (Ra7,Rb7,X2,Z16), (Ra7,Rb7,X2,Z17), (Ra7,Rb7,X2,Z18), (Ra7,Rb7,X2,Z19), (Ra7,Rb7,X2,Z20), (Ra7,Rb7,X2,Z21), (Ra7,Rb7,X2,Z22), (Ra7,Rb7,X2,Z23), (Ra7,Rb7,X2,Z24), (Ra7,Rb7,X2,Z25), (Ra7,Rb7,X2,Z26), (Ra7,Rb7,X2,Z27), (Ra7,Rb7,X2,Z28), (Ra7,Rb7,X2,Z29), (Ra7,Rb7,X2,Z30), (Ra7,Rb7,X2,Z31), (Ra7,Rb7,X2,Z32), (Ra7,Rb7,X2,Z33), (Ra7,Rb7,X2,Z34), (Ra7,Rb7,X2,Z35), (Ra7,Rb7,X2,Z36), (Ra7,Rb7,X2,Z37), (Ra7,Rb7,X2,Z38), (Ra7,Rb7,X2,Z39), (Ra7,Rb8,X1,Z1), (Ra7,Rb8,X1,Z2), (Ra7,Rb8,X1,Z3), (Ra7,Rb8,X1,Z4), (Ra7,Rb8,X1,Z5), (Ra7,Rb8,X1,Z6), (Ra7,Rb8,X1,Z7), (Ra7,Rb8,X1,Z8), (Ra7,Rb8,X1,Z9), (Ra7,Rb8,X1,Z10), (Ra7,Rb8,X1,Z11), (Ra7,Rb8,X1,Z12), (Ra7,Rb8,X1,Z13), (Ra7,Rb8,X1,Z14), (Ra7,Rb8,X1,Z15), (Ra7,Rb8,X1,Z16), (Ra7,Rb8,X1,Z17), (Ra7,Rb8,X1,Z18), (Ra7,Rb8,X1,Z19), (Ra7,Rb8,X1,Z20), (Ra7,Rb8,X1,Z21), (Ra7,Rb8,X1,Z22), (Ra7,Rb8,X1,Z23), (Ra7,Rb8,X1,Z24), (Ra7,Rb8,Z25), (Ra7,Rb8,X1,Z26), (Ra7,Rb8,X1,Z27), (Ra7,Rb8,X1,Z28), (Ra7,Rb8,X1,Z29), (Ra7,Rb8,X1,Z30), (Ra7,Rb8,X1,Z31), (Ra7,Rb8,X1,Z32), (Ra7,Rb8,X1,Z33), (Ra7,Rb8,X1,Z34), (Ra7,Rb8,X1,Z35), (Ra7,Rb8,X1,Z36), (Ra7,Rb8,X1,Z37), (Ra7,Rb8,X1,Z38), (Ra7,Rb8,X1,Z39), (Ra7,Rb8,X2,Z1), (Ra7,Rb8,X2,Z2), (Ra7,Rb8,X2,Z3), (Ra7,Rb8,X2,Z4), (Ra7,Rb8,X2,Z5), (Ra7,Rb8,X2,Z6), (Ra7,Rb8,X2,Z7), (Ra7,Rb8,X2,Z8), (Ra7,Rb8,X2,Z9), (Ra7,Rb8,X2,Z10), (Ra7,Rb8,X2,Z11), (Ra7,Rb8,X2,Z12), (Ra7,Rb8,X2,Z13), (Ra7,Rb8,X2,Z14), (Ra7,Rb8,X2,Z15), (Ra7,Rb8,X2,Z16), (Ra7,Rb8,X2,Z17), (Ra7,Rb8,X2,Z18), (Ra7,Rb8,X2,Z19), (Ra7,Rb8,X2,Z20), (Ra7,Rb8,X2,Z21), (Ra7,Rb8,X2,Z22), (Ra7,Rb8,X2,Z23), (Ra7,Rb8,X2,Z24), (Ra7,Rb8,X2,Z25), (Ra7,Rb8,X2,Z26), (Ra7,Rb8,X2,Z27), (Ra7,Rb8,X2,Z28), (Ra7,Rb8,X2,Z29), (Ra7,Rb8,X2,Z30), (Ra7,Rb8,X2,Z31), (Ra7,Rb8,X2,Z32), (Ra7,Rb8,X2,Z33), (Ra7,Rb8,X2,Z34), (Ra7,Rb8,X2,Z35), (Ra7,Rb8,X2,Z36), (Ra7,Rb8,X2,Z37), (Ra7,Rb8,X2,Z38), (Ra7,Rb8,X2,Z39), (Ra8,Rb1,X1,Z1), (Ra8,Rb1,X1,Z2), (Ra8,Rb1,X1,Z3), (Ra8,Rb1,X1,Z4), (Ra8,Rb1,X1,Z5), (Ra8,Rb1,X1,Z6), (Ra8,Rb1,X1,Z7), (Ra8,Rb1,X1,Z8), (Ra8,Rb1,X1,Z9), (Ra8,Rb1,X1,Z10), (Ra8,Rb1,X1,Z11), (Ra8,Rb1,X1,Z12), (Ra8,Rb1,X1,Z13), (Ra8,Rb1,X1,Z14), (Ra8,Rb1,X1,Z15), (Ra8,Rb1,X1,Z16), (Ra8,Rb1,X1,Z17), (Ra8,Rb1,X1,Z18), (Ra8,Rb1,X1,Z19), (Ra8,Rb1,X1,Z20), (Ra8,Rb1,X1,Z21), (Ra8,Rb1,X1,Z22), (Ra8,Rb1,X1,Z23), (Ra8,Rb1,X1,Z24), (Ra8,Rb1,X1,Z25), (Ra8,Rb1,X1,Z26), (Ra8,Rb1,X1,Z27), (Ra8,Rb1,X1,Z28), (Ra8,Rb1,X1,Z29), (Ra8,Rb1,X1,Z30), (Ra8,Rb1,X1,Z31), (Ra8,Rb1,X1,Z32), (Ra8,Rb1,X1,Z33), (Ra8,Rb1,X1,Z34), (Ra8,Rb1,X1,Z35), (Ra8,Rb1,X1,Z36), (Ra8,Rb1,X1,Z37), (Ra8,Rb1,X1,Z38), (Ra8,Rb1,X1,Z39), (Ra8,Rb1,X2,Z1), (Ra8,Rb1,X2,Z2), (Ra8,Rb1,X2,Z3), (Ra8,Rb1,X2,Z4), (Ra8,Rb1,X2,Z5), (Ra8,Rb1,X2,Z6), (Ra8,Rb1,X2,Z7), (Ra8,Rb1,X2,Z8), (Ra8,Rb1,X2,Z9), (Ra8,Rb1,X2,Z10), (Ra8,Rb1,X2,Z11), (Ra8,Rb1,X2,Z12), (Ra8,Rb1,X2,Z13), (Ra8,Rb1,X2,Z14), (Ra8,Rb1,X2,Z15), (Ra8,Rb1,X2,Z16), (Ra8,Rb1,X2,Z17), (Ra8,Rb1,X2,Z18), (Ra8,Rb1,X2,Z19), (Ra8,Rb1,X2,Z20), (Ra8,Rb1,X2,Z21), (Ra8,Rb1,X2,Z22), (Ra8,Rb1,X2,Z23), (Ra8,Rb1,X2,Z24), (Ra8,Rb1,X2,Z25), (Ra8,Rb1,X2,Z26), (Ra8,Rb1,X2,Z27), (Ra8,Rb1,X2,Z28), (Ra8,Rb1,X2,Z29), (Ra8,Rb1,X2,Z30), (Ra8,Rb1,X2,Z31), (Ra8,Rb1,X2,Z32), (Ra8,Rb1,X2,Z33), (Ra8,Rb1,X2,Z34), (Ra8,Rb1,X2,Z35), (Ra8,Rb1,X2,Z36), (Ra8,Rb1,X2,Z37), (Ra8,Rb1,X2,Z38), (Ra8,Rb1,X2,Z39), (Ra8,Rb2,X1,Z1), (Ra8,Rb2,X1,Z2), (Ra8,Rb2,X1,Z3), (Ra8,Rb2,X1,Z4), (Ra8,Rb2,X1,Z5), (Ra8,Rb2,X1,Z6), (Ra8,Rb2,X1,Z7), (Ra8,Rb2,X1,Z8), (Ra8,Rb2,X1,Z9), (Ra8,Rb2,X1,Z10), (Ra8,Rb2,X1,Z11), (Ra8,Rb2,X1,Z12), (Ra8,Rb2,X1,Z13), (Ra8,Rb2,X1,Z14), (Ra8,Rb2,X1,Z15), (Ra8,Rb2,X1,Z16), (Ra8,Rb2,X1,Z17), (Ra8,Rb2,X1,Z18), (Ra8,Rb2,X1,Z19), (Ra8,Rb2,X1,Z20), (Ra8,Rb2,X1,Z21), (Ra8,Rb2,X1,Z22), (Ra8,Rb2,X1,Z23), (Ra8,Rb2,X1,Z24), (Ra8,Rb2,X1,Z25), (Ra8,Rb2,X1,Z26), (Ra8,Rb2,X1,Z27), (Ra8,Rb2,X1,Z28), (Ra8,Rb2,X1,Z29), (Ra8,Rb2,X1,Z30), (Ra8,Rb2,X1,Z31), (Ra8,Rb2,X1,Z32), (Ra8,Rb2,X1,Z33), (Ra8,Rb2,X1,Z34), (Ra8,Rb2,X1,Z35), (Ra8,Rb2,X1,Z36), (Ra8,Rb2,X1,Z37), (Ra8,Rb2,X1,Z38), (Ra8,Rb2,X1,Z39), (Ra8,Rb2,X2,Z1), (Ra8,Rb2,X2,Z2), (Ra8,Rb2,X2,Z3), (Ra8,Rb2,X2,Z4), (Ra8,Rb2,X2,Z5), (Ra8,Rb2,X2,Z6), (Ra8,Rb2,X2,Z7), (Ra8,Rb2,X2,Z8), (Ra8,Rb2,X2,Z9), (Ra8,Rb2,X2,Z10), (Ra8,Rb2,X2,Z11), (Ra8,Rb2,X2,Z12), (Ra8,Rb2,X2,Z13), (Ra8,Rb2,X2,Z14), (Ra8,Rb2,X2,Z15), (Ra8,Rb2,X2,Z16), (Ra8,Rb2,X2,Z17), (Ra8,Rb2,X2,Z18), (Ra8,Rb2,X2,Z19), (Ra8,Rb2,X2,Z20), (Ra8,Rb2,X2,Z21), (Ra8,Rb2,X2,Z22), (Ra8,Rb2,X2,Z23), (Ra8,Rb2,X2,Z24), (Ra8,Rb2,X2,Z25), (Ra8,Rb2,X2,Z26), (Ra8,Rb2,X2,Z27), (Ra8,Rb2,X2,Z28), (Ra8,Rb2,X2,Z29), (Ra8,Rb2,X2,Z30), (Ra8,Rb2,X2,Z31), (Ra8,Rb2,X2,Z32), (Ra8,Rb2,X2,Z33), (Ra8,Rb2,X2,Z34), (Ra8,Rb2,X2,Z35), (Ra8,Rb2,X2,Z36), (Ra8,Rb2,X2,Z37), (Ra8,Rb2,X2,Z38), (Ra8,Rb2,X2,Z39), (Ra8,Rb3,X1,Z1), (Ra8,Rb3,X1,Z2), (Ra8,Rb3,X1,Z3), (Ra8,Rb3,X1,Z4), (Ra8,Rb3,X1,Z5), (Ra8,Rb3,X1,Z6), (Ra8,Rb3,X1,Z7), (Ra8,Rb3,X1,Z8), (Ra8,Rb3,X1,Z9), (Ra8,Rb3,X1,Z10), (Ra8,Rb3,X1,Z11), (Ra8,Rb3,X1,Z12), (Ra8,Rb3,X1,Z13), (Ra8,Rb3,X1,Z14), (Ra8,Rb3,X1,Z15), (Ra8,Rb3,X1,Z16), (Ra8,Rb3,X1,Z17), (Ra8,Rb3,X1,Z18), (Ra8,Rb3,X1,Z19), (Ra8,Rb3,X1,Z20), (Ra8,Rb3,X1,Z21), (Ra8,Rb3,X1,Z22), (Ra8,Rb3,X1,Z23), (Ra8,Rb3,X1,Z24), (Ra8,Rb3,X1,Z25), (Ra8,Rb3,X1,Z26), (Ra8,Rb3,X1,Z27), (Ra8,Rb3,X1,Z28), (Ra8,Rb3,X1,Z29), (Ra8,Rb3,X1,Z30), (Ra8,Rb3,X1,Z31), (Ra8,Rb3,X1,Z32), (Ra8,Rb3,X1,Z33), (Ra8,Rb3,X1,Z34), (Ra8,Rb3,X1,Z35), (Ra8,Rb3,X1,Z36), (Ra8,Rb3,X1,Z37), (Ra8,Rb3,X1,Z38), (Ra8,Rb3,X1,Z39), (Ra8,Rb3,X2,Z1), (Ra8,Rb3,X2,Z2), (Ra8,Rb3,X2,Z3), (Ra8,Rb3,X2,Z4), (Ra8,Rb3,X2,Z5), (Ra8,Rb3,X2,Z6), (Ra8,Rb3,X2,Z7), (Ra8,Rb3,X2,Z8), (Ra8,Rb3,X2,Z9), (Ra8,Rb3,X2,Z10), (Ra8,Rb3,X2,Z11), (Ra8,Rb3,X2,Z12), (Ra8,Rb3,X2,Z13), (Ra8,Rb3,X2,Z14), (Ra8,Rb3,X2,Z15), (Ra8,Rb3,X2,Z16), (Ra8,Rb3,X2,Z17), (Ra8,Rb3,X2,Z18), (Ra8,Rb3,X2,Z19), (Ra8,Rb3,X2,Z20), (Ra8,Rb3,X2,Z21), (Ra8,Rb3,X2,Z22), (Ra8,Rb3,X2,Z23), (Ra8,Rb3,X2,Z24), (Ra8,Rb3,X2,Z25), (Ra8,Rb3,X2,Z26), (Ra8,Rb3,X2,Z27), (Ra8,Rb3,X2,Z28), (Ra8,Rb3,X2,Z29), (Ra8,Rb3,X2,Z30), (Ra8,Rb3,X2,Z31), (Ra8,Rb3,X2,Z32), (Ra8,Rb3,X2,Z33), (Ra8,Rb3,X2,Z34), (Ra8,Rb3,X2,Z35), (Ra8,Rb3,X2,Z36), (Ra8,Rb3,X2,Z37), (Ra8,Rb3,X2,Z38), (Ra8,Rb3,X2,Z39), (Ra8,Rb4,X1,Z1), (Ra8,Rb4,X1,Z2), (Ra8,Rb4,X1,Z3), (Ra8,Rb4,X1,Z4), (Ra8,Rb4,X1,Z5), (Ra8,Rb4,X1,Z6), (Ra8,Rb4,X1,Z7), (Ra8,Rb4,X1,Z8), (Ra8,Rb4,X1,Z9), (Ra8,Rb4,X1,Z10), (Ra8,Rb4,X1,Z11), (Ra8,Rb4,X1,Z12), (Ra8,Rb4,X1,Z13), (Ra8,Rb4,X1,Z14), (Ra8,Rb4,X1,Z15), (Ra8,Rb4,X1,Z16), (Ra8,Rb4,X1,Z17), (Ra8,Rb4,X1,Z18), (Ra8,Rb4,X1,Z19), (Ra8,Rb4,X1,Z20), (Ra8,Rb4,X1,Z21), (Ra8,Rb4,X1,Z22), (Ra8,Rb4,X1,Z23), (Ra8,Rb4,X1,Z24), (Ra8,Rb4,X1,Z25), (Ra8,Rb4,X1,Z26), (Ra8,Rb4,X1,Z27), (Ra8,Rb4,X1,Z28), (Ra8,Rb4,X1,Z29), (Ra8,Rb4,X1,Z30), (Ra8,Rb4,X1,Z31), (Ra8,Rb4,X1,Z32), (Ra8,Rb4,X1,Z33), (Ra8,Rb4,X1,Z34), (Ra8,Rb4,X1,Z35), (Ra8,Rb4,X1,Z36), (Ra8,Rb4,X1,Z37), (Ra8,Rb4,X1,Z38), (Ra8,Rb4,X1,Z39), (Ra8,Rb4,X2,Z1), (Ra8,Rb4,X2,Z2), (Ra8,Rb4,X2,Z3), (Ra8,Rb4,X2,Z4), (Ra8,Rb4,X2,Z5), (Ra8,Rb4,X2,Z6), (Ra8,Rb4,X2,Z7), (Ra8,Rb4,X2,Z8), (Ra8,Rb4,X2,Z9), (Ra8,Rb4,X2,Z10), (Ra8,Rb4,X2,Z11), (Ra8,Rb4,X2,Z12), (Ra8,Rb4,X2,Z13), (Ra8,Rb4,X2,Z14), (Ra8,Rb4,X2,Z15), (Ra8,Rb4,X2,Z16), (Ra8,Rb4,X2,Z17), (Ra8,Rb4,X2,Z18), (Ra8,Rb4,X2,Z19), (Ra8,Rb4,X2,Z20), (Ra8,Rb4,X2,Z21), (Ra8,Rb4,X2,Z22), (Ra8,Rb4,X2,Z23), (Ra8,Rb4,X2,Z24), (Ra8,Rb4,X2,Z25), (Ra8,Rb4,X2,Z26), (Ra8,Rb4,X2,Z27), (Ra8,Rb4,X2,Z28), (Ra8,Rb4,X2,Z29), (Ra8,Rb4,X2,Z30), (Ra8,Rb4,X2,Z31), (Ra8,Rb4,X2,Z32), (Ra8,Rb4,X2,Z33), (Ra8,Rb4,X2,Z34), (Ra8,Rb4,X2,Z35), (Ra8,Rb4,X2,Z36), (Ra8,Rb4,X2,Z37), (Ra8,Rb4,X2,Z38), (Ra8,Rb4,X2,Z39), (Ra8,Rb5,X1,Z1), (Ra8,Rb5,X1,Z2), (Ra8,Rb5,X1,Z3), (Ra8,Rb5,X1,Z4), (Ra8,Rb5,X1,Z5), (Ra8,Rb5,X1,Z6), (Ra8,Rb5,X1,Z7), (Ra8,Rb5,X1,Z8), (Ra8,Rb5,X1,Z9), (Ra8,Rb5,X1,Z10), (Ra8,Rb5,X1,Z11), (Ra8,Rb5,X1,Z12), (Ra8,Rb5,X1,Z13), (Ra8,Rb5,X1,Z14), (Ra8,Rb5,X1,Z15), (Ra8,Rb5,X1,Z16), (Ra8,Rb5,X1,Z17), (Ra8,Rb5,X1,Z18), (Ra8,Rb5,X1,Z19), (Ra8,Rb5,X1,Z20), (Ra8,Rb5,X1,Z21), (Ra8,Rb5,X1,Z22), (Ra8,Rb5,X1,Z23), (Ra8,Rb5,X1,Z24), (Ra8,Rb5,X1,Z25), (Ra8,Rb5,X1,Z26), (Ra8,Rb5,X1,Z27), (Ra8,Rb5,X1,Z28), (Ra8,Rb5,X1,Z29), (Ra8,Rb5,X1,Z30), (Ra8,Rb5,X1,Z31), (Ra8,Rb5,X1,Z32), (Ra8,Rb5,X1,Z33), (Ra8,Rb5,X1,Z34), (Ra8,Rb5,X1,Z35), (Ra8,Rb5,X1,Z36), (Ra8,Rb5,X1,Z37), (Ra8,Rb5,X1,Z38), (Ra8,Rb5,X1,Z39), (Ra8,Rb5,X2,Z1), (Ra8,Rb5,X2,Z2), (Ra8,Rb5,X2,Z3), (Ra8,Rb5,X2,Z4), (Ra8,Rb5,X2,Z5), (Ra8,Rb5,X2,Z6), (Ra8,Rb5,X2,Z7), (Ra8,Rb5,X2,Z8), (Ra8,Rb5,X2,Z9), (Ra8,Rb5,X2,Z10), (Ra8,Rb5,X2,Z11), (Ra8,Rb5,X2,Z12), (Ra8,Rb5,X2,Z13), (Ra8,Rb5,X2,Z14), (Ra8,Rb5,X2,Z15), (Ra8,Rb5,X2,Z16), (Ra8,Rb5,X2,Z17), (Ra8,Rb5,X2,Z18), (Ra8,Rb5,X2,Z19), (Ra8,Rb5,X2,Z20), (Ra8,Rb5,X2,Z21), (Ra8,Rb5,X2,Z22), (Ra8,Rb5,X2,Z23), (Ra8,Rb5,X2,Z24), (Ra8,Rb5,X2,Z25), (Ra8,Rb5,X2,Z26), (Ra8,Rb5,X2,Z27), (Ra8,Rb5,X2,Z28), (Ra8,Rb5,X2,Z29), (Ra8,Rb5,X2,Z30), (Ra8,Rb5,X2,Z31), (Ra8,Rb5,X2,Z32), (Ra8,Rb5,X2,Z33), (Ra8,Rb5,X2,Z34), (Ra8,Rb5,X2,Z35), (Ra8,Rb5,X2,Z36), (Ra8,Rb5,X2,Z37), (Ra8,Rb5,X2,Z38), (Ra8,Rb5,X2,Z39), (Ra8,Rb6,X1,Z1), 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(Ra8,Rb6,X2,Z19), (Ra8,Rb6,X2,Z20), (Ra8,Rb6,X2,Z21), (Ra8,Rb6,X2,Z22), (Ra8,Rb6,X2,Z23), (Ra8,Rb6,X2,Z24), (Ra8,Rb6,X2,Z25), (Ra8,Rb6,X2,Z26), (Ra8,Rb6,X2,Z27), (Ra8,Rb6,X2,Z28), (Ra8,Rb6,X2,Z29), (Ra8,Rb6,X2,Z30), (Ra8,Rb6,X2,Z31), (Ra8,Rb6,X2,Z32), (Ra8,Rb6,X2,Z33), (Ra8,Rb6,X2,Z34), (Ra8,Rb6,X2,Z35), (Ra8,Rb6,X2,Z36), (Ra8,Rb6,X2,Z37), (Ra8,Rb6,X2,Z38), (Ra8,Rb6,X2,Z39), (Ra8,Rb7,X1,Z1), (Ra8,Rb7,X1,Z2), (Ra8,Rb7,X1,Z3), (Ra8,Rb7,X1,Z4), (Ra8,Rb7,X1,Z5), (Ra8,Rb7,X1,Z6), (Ra8,Rb7,X1,Z7), (Ra8,Rb7,X1,Z8), (Ra8,Rb7,X1,Z9), (Ra8,Rb7,X1,Z10), (Ra8,Rb7,X1,Z11), (Ra8,Rb7,X1,Z12), (Ra8,Rb7,X1,Z13), (Ra8,Rb7,X1,Z14), (Ra8,Rb7,X1,Z15), (Ra8,Rb7,X1,Z16), (Ra8,Rb7,X1,Z17), (Ra8,Rb7,X1,Z18), (Ra8,Rb7,X1,Z19), (Ra8,Rb7,X1,Z20), (Ra8,Rb7,X1,Z21), (Ra8,Rb7,X1,Z22), (Ra8,Rb7,X1,Z23), (Ra8,Rb7,X1,Z24), (Ra8,Rb7,X1,Z25), (Ra8,Rb7,X1,Z26), (Ra8,Rb7,X1,Z27), (Ra8,Rb7,X1,Z28), (Ra8,Rb7,X1,Z29), (Ra8,Rb7,X1,Z30), (Ra8,Rb7,X1,Z31), (Ra8,Rb7,X1,Z32), (Ra8,Rb7,X1,Z33), (Ra8,Rb7,X1,Z34), (Ra8,Rb7,X1,Z35), 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(Ra11,Rb6,X1,Z31), (Ra11,Rb6,X1,Z32), (Ra11,Rb6,X1,Z33), (Ra11,Rb6,X1,Z34), (Ra11,Rb6,X1,Z35), (Ra11,Rb6,X1,Z36), (Ra11,Rb6,X1,Z37), (Ra11,Rb6,X1,Z38), (Ra11,Rb6,X1,Z39), (Ra11,Rb6,X2,Z1), (Ra11,Rb6,X2,Z2), (Ra11,Rb6,X2,Z3), (Ra11,Rb6,X2,Z4), (Ra11,Rb6,X2,Z5), (Ra11,Rb6,X2,Z6), (Ra11,Rb6,X2,Z7), (Ra11,Rb6,X2,Z8), (Ra11,Rb6,X2,Z9), (Ra11,Rb6,X2,Z10), (Ra11,Rb6,X2,Z11), (Ra11,Rb6,X2,Z12), (Ra11,Rb6,X2,Z13), (Ra11,Rb6,X2,Z14), (Ra11,Rb6,X2,Z15), (Ra11,Rb6,X2,Z16), (Ra11,Rb6,X2,Z17), (Ra11,Rb6,X2,Z18), (Ra11,Rb6,X2,Z19), (Ra11,Rb6,X2,Z20), (Ra11,Rb6,X2,Z21), (Ra11,Rb6,X2,Z22), (Ra11,Rb6,X2,Z23), (Ra11,Rb6,X2,Z24), (Ra11,Rb6,X2,Z25), (Ra11,Rb6,X2,Z26), (Ra11,Rb6,X2,Z27), (Ra11,Rb6,X2,Z28), (Ra11,Rb6,X2,Z29), (Ra11,Rb6,X2,Z30), (Ra11,Rb6,X2,Z31), (Ra11,Rb6,X2,Z32), (Ra11,Rb6,X2,Z33), (Ra11,Rb6,X2,Z34), (Ra11,Rb6,X2,Z35), (Ra11,Rb6,X2,Z36), (Ra11,Rb6,X2,Z37), (Ra11,Rb6,X2,Z38), (Ra11,Rb6,X2,Z39), (Ra11,Rb7,X1,Z1), (Ra11,Rb7,X1,Z2), (Ra11,Rb7,X1,Z3), (Ra11,Rb7,X1,Z4), (Ra11,Rb7,X1,Z5), (Ra11,Rb7,X1,Z6), (Ra11,Rb7,X1,Z7), (Ra11,Rb7,X1,Z8), (Ra11,Rb7,X1,Z9), (Ra11,Rb7,X1,Z10), (Ra11,Rb7,X1,Z11), (Ra11,Rb7,X1,Z12), (Ra11,Rb7,X1,Z13), (Ra11,Rb7,X1,Z14), (Ra11,Rb7,X1,Z15), (Ra11,Rb7,X1,Z16), (Ra11,Rb7,X1,Z17), (Ra11,Rb7,X1,Z18), (Ra11,Rb7,X1,Z19), (Ra11,Rb7,X1,Z20), (Ra11,Rb7,X1,Z21), (Ra11,Rb7,X1,Z22), (Ra11,Rb7,X1,Z23), (Ra11,Rb7,X1,Z24), (Ra11,Rb7,X1,Z25), (Ra11,Rb7,X1,Z26), (Ra11,Rb7,X1,Z27), (Ra11,Rb7,X1,Z28), (Ra11,Rb7,X1,Z29), (Ra11,Rb7,X1,Z30), (Ra11,Rb7,X1,Z31), (Ra11,Rb7,X1,Z32), (Ra11,Rb7,X1,Z33), (Ra11,Rb7,X1,Z34), (Ra11,Rb7,X1,Z35), (Ra11,Rb7,X1,Z36), (Ra11,Rb7,X1,Z37), (Ra11,Rb7,X1,Z38), (Ra11,Rb7,X1,Z39), (Ra11,Rb7,X2,Z1), (Ra11,Rb7,X2,Z2), (Ra11,Rb7,X2,Z3), (Ra11,Rb7,X2,Z4), (Ra11,Rb7,X2,Z5), (Ra11,Rb7,X2,Z6), (Ra11,Rb7,X2,Z7), (Ra11,Rb7,X2,Z8), (Ra11,Rb7,X2,Z9), (Ra11,Rb7,X2,Z10), (Ra11,Rb7,X2,Z11), (Ra11,Rb7,X2,Z12), (Ra11,Rb7,X2,Z13), (Ra11,Rb7,X2, Z14), (Ra11,Rb7,X2,Z15), (Ra11,Rb7,X2,Z16), (Ra11,Rb7,X2,Z17), (Ra11,Rb7,X2,Z18), (Ra11,Rb7,X2,Z19), 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(Ra12,Rb1,X1,Z9), (Ra12,Rb1,X1,Z10), (Ra12,Rb1,X1,Z11), (Ra12,Rb1,X1,Z12), (Ra12,Rb1,X1,Z13), (Ra12,Rb1,X1,Z14), (Ra12,Rb1,X1,Z15), (Ra12,Rb1,X1,Z16), (Ra12,Rb1,X1,Z17), (Ra12,Rb1,X1,Z18), (Ra12,Rb1,X1,Z19), (Ra12,Rb1,X1,Z20), (Ra12,Rb1,X1,Z21), (Ra12,Rb1,X1,Z22), (Ra12,Rb1,X1,Z23), (Ra12,Rb1,X1,Z24), (Ra12,Rb1,X1,Z25), (Ra12,Rb1,X1,Z26), (Ra12,Rb1,X1,Z27), (Ra12,Rb1,X1,Z28), (Ra12,Rb1,X1,Z29), (Ra12,Rb1,X1,Z30), (Ra12,Rb1,X1,Z31), (Ra12,Rb1,X1,Z32), (Ra12,Rb1,X1,Z33), (Ra12,Rb1,X1,Z34), (Ra12,Rb1,X1,Z35), (Ra12,Rb1,X1,Z36), (Ra12,Rb1,X1,Z37), (Ra12,Rb1,X1,Z38), (Ra12,Rb1,X1,Z39), (Ra12,Rb1,X2,Z1), (Ra12,Rb1,X2,Z2), (Ra12,Rb1,X2,Z3), (Ra12,Rb1,X2,Z4), (Ra12,Rb1,X2,Z5), (Ra12,Rb1,X2,Z6), (Ra12,Rb1,X2,Z7), (Ra12,Rb1,X2,Z8), (Ra12,Rb1,X2,Z9), (Ra12,Rb1,X2,Z10), (Ra12,Rb1,X2,Z11), (Ra12,Rb1,X2,Z12), (Ra12,Rb1,X2,Z13), (Ra12,Rb1,X2,Z14), (Ra12,Rb1,X2,Z15), (Ra12,Rb1,X2,Z16), (Ra12,Rb1,X2,Z17), (Ra12,Rb1,X2,Z18), (Ra12,Rb1,X2,Z19), (Ra12,Rb1,X2,Z20), (Ra12,Rb1,X2,Z21), (Ra12,Rb1,X2,Z22), (Ra12,Rb1,X2,Z23), (Ra12,Rb1,X2,Z24), (Ra12,Rb1,X2,Z25), (Ra12,Rb1,X2,Z26), (Ra12,Rb1,X2,Z27), (Ra12,Rb1,X2,Z28), (Ra12,Rb1,X2,Z29), (Ra12,Rb1,X2,Z30), (Ra12,Rb1,X2,Z31), (Ra12,Rb1,X2,Z32), (Ra12,Rb1,X2,Z33), (Ra12,Rb1,X2,Z34), (Ra12,Rb1,X2,Z35), (Ra12,Rb1,X2,Z36), (Ra12,Rb1,X2,Z37), (Ra12,Rb1,X2,Z38), (Ra12,Rb1,X2,Z39), (Ra12,Rb2,X1,Z1), (Ra12,Rb2,X1,Z2), (Ra12,Rb2,X1,Z3), (Ra12,Rb2,X1,Z4), (Ra12,Rb2,X1,Z5), (Ra12,Rb2,X1,Z6), (Ra12,Rb2,X1,Z7), (Ra12,Rb2,X1,Z8), (Ra12,Rb2,X1,Z9), (Ra12,Rb2,X1,Z10), (Ra12,Rb2,X1,Z11), (Ra12,Rb2,X1,Z12), (Ra12,Rb2,X1,Z13), (Ra12,Rb2,X1,Z14), (Ra12,Rb2,X1,Z15), (Ra12,Rb2,X1,Z16), (Ra12,Rb2,X1,Z17), (Ra12,Rb2,X1,Z18), (Ra12,Rb2,X1,Z19), (Ra12,Rb2,X1,Z20), (Ra12,Rb2,X1,Z21), (Ra12,Rb2,X1,Z22), (Ra12,Rb2,X1,Z23), (Ra12,Rb2,X1,Z24), (Ra12,Rb2,X1,Z25), (Ra12,Rb2,X1,Z26), (Ra12,Rb2,X1,Z27), (Ra12,Rb2,X1,Z28), (Ra12,Rb2,X1,Z29), (Ra12,Rb2,X1,Z30), (Ra12,Rb2,X1,Z31), (Ra12,Rb2,X1,Z32), (Ra12,Rb2,X1,Z33), (Ra12,Rb2,X1,Z34), (Ra12,Rb2,X1,Z35), (Ra12,Rb2,X1,Z36), (Ra12,Rb2,X1,Z37), (Ra12,Rb2,X1,Z38), (Ra12,Rb2,X1,Z39), (Ra12,Rb2,X2,Z1), (Ra12,Rb2,X2,Z2), (Ra12,Rb2,X2,Z3), (Ra12,Rb2,X2,Z4), (Ra12,Rb2,X2,Z5), (Ra12,Rb2,X2,Z6), (Ra12,Rb2,X2,Z7), (Ra12,Rb2,X2,Z8), (Ra12,Rb2,X2,Z9), (Ra12,Rb2,X2,Z10), (Ra12,Rb2,X2,Z11), (Ra12,Rb2,X2,Z12), (Ra12,Rb2,X2,Z13), (Ra12,Rb2,X2,Z14), (Ra12,Rb2,X2,Z15), (Ra12,Rb2,X2,Z16), (Ra12,Rb2,X2,Z17), (Ra12,Rb2,X2, Z18), (Ra12,Rb2,X2,Z19), (Ra12,Rb2,X2,Z20), (Ra12,Rb2,X2,Z21), (Ra12,Rb2,X2,Z22), (Ra12,Rb2,X2,Z23), (Ra12,Rb2,X2,Z24), (Ra12,Rb2,X2,Z25), (Ra12,Rb2,X2,Z26), (Ra12,Rb2,X2,Z27), (Ra12,Rb2,X2,Z28), (Ra12,Rb2,X2,Z29), (Ra12,Rb2,X2,Z30), (Ra12,Rb2,X2,Z31), (Ra12,Rb2,X2,Z32), (Ra12,Rb2,X2,Z33), (Ra12,Rb2,X2,Z34), (Ra12,Rb2,X2,Z35), (Ra12,Rb2,X2,Z36), (Ra12,Rb2,X2,Z37), (Ra12,Rb2,X2,Z38), (Ra12,Rb2,X2,Z39), (Ra12,Rb3,X1,Z1), (Ra12,Rb3,X1,Z2), (Ra12,Rb3,X1,Z3), (Ra12,Rb3,X1,Z4), (Ra12,Rb3,X1,Z5), (Ra12,Rb3,X1,Z6), (Ra12,Rb3,X1,Z7), (Ra12,Rb3,X1,Z8), (Ra12,Rb3,X1,Z9), (Ra12,Rb3,X1,Z10), (Ra12,Rb3,X1,Z11), (Ra12,Rb3,X1,Z12), (Ra12,Rb3,X1,Z13), (Ra12,Rb3,X1,Z14), (Ra12,Rb3,X1,Z15), (Ra12,Rb3,X1,Z16), (Ra12,Rb3,X1,Z17), (Ra12,Rb3,X1,Z18), (Ra12,Rb3,X1,Z19), (Ra12,Rb3,X1,Z20), (Ra12,Rb3,X1,Z21), (Ra12,Rb3,X1,Z22), (Ra12,Rb3,X1,Z23), (Ra12,Rb3,X1,Z24), (Ra12,Rb3,X1,Z25), (Ra12,Rb3,X1,Z26), (Ra12,Rb3,X1,Z27), (Ra12,Rb3,X1,Z28), (Ra12,Rb3,X1,Z29), (Ra12,Rb3,X1,Z30), (Ra12,Rb3,X1,Z31), (Ra12,Rb3,X1,Z32), (Ra12,Rb3,X1,Z33), (Ra12,Rb3,X1,Z34), (Ra12,Rb3,X1,Z35), (Ra12,Rb3,X1,Z36), (Ra12,Rb3,X1,Z37), (Ra12,Rb3,X1,Z38), (Ra12,Rb3,X1,Z39), (Ra12,Rb3,X2,Z1), (Ra12,Rb3,X2,Z2), (Ra12,Rb3,X2,Z3), (Ra12,Rb3,X2,Z4), (Ra12,Rb3,X2,Z5), (Ra12,Rb3,X2,Z6), (Ra12,Rb3,X2,Z7), (Ra12,Rb3,X2,Z8), (Ra12,Rb3,X2,Z9), (Ra12,Rb3,X2,Z10), (Ra12,Rb3,X2,Z11), (Ra12,Rb3,X2,Z12), (Ra12,Rb3,X2,Z13), (Ra12,Rb3,X2,Z14), (Ra12,Rb3,X2,Z15), (Ra12,Rb3,X2,Z16), (Ra12,Rb3,X2,Z17), (Ra12,Rb3,X2,Z18), (Ra12,Rb3,X2,Z19), (Ra12,Rb3,X2,Z20), (Ra12, Rb3,X2,Z21), (Ra12,Rb3,X2,Z22), (Ra12,Rb3,X2,Z23), (Ra12,Rb3,X2,Z24), (Ra12,Rb3,X2,Z25), (Ra12,Rb3,X2,Z26), (Ra12,Rb3,X2,Z27), (Ra12,Rb3,X2,Z28), (Ra12,Rb3,X2,Z29), (Ra12,Rb3,X2,Z30), (Ra12,Rb3,X2,Z31), (Ra12,Rb3,X2,Z32), (Ra12,Rb3,X2,Z33), (Ra12,Rb3,X2,Z34), (Ra12,Rb3,X2,Z35), (Ra12,Rb3,X2,Z36), (Ra12,Rb3,X2,Z37), (Ra12,Rb3,X2,Z38), (Ra12,Rb3,X2,Z39), (Ra12,Rb4,X1,Z1), (Ra12,Rb4,X1,Z2), (Ra12,Rb4,X1,Z3), (Ra12,Rb4,X1,Z4), (Ra12,Rb4,X1,Z5), (Ra12,Rb4,X1,Z6), (Ra12,Rb4,X1,Z7), (Ra12,Rb4,X1,Z8), (Ra12,Rb4,X1,Z9), (Ra12,Rb4,X1,Z10), (Ra12,Rb4,X1,Z11), (Ra12,Rb4,X1,Z12), (Ra12,Rb4,X1,Z13), (Ra12,Rb4,X1,Z14), (Ra12,Rb4,X1,Z15), (Ra12,Rb4,X1,Z16), (Ra12,Rb4,X1,Z17), (Ra12,Rb4,X1,Z18), (Ra12,Rb4,X1,Z19), (Ra12,Rb4,X1,Z20), (Ra12,Rb4,X1,Z21), (Ra12,Rb4,X1,Z22), (Ra12,Rb4,X1,Z23), (Ra12,Rb4,X1,Z24), (Ra12,Rb4,X1,Z25), (Ra12,Rb4,X1,Z26), (Ra12,Rb4,X1,Z27), (Ra12,Rb4,X1,Z28), (Ra12,Rb4,X1,Z29), (Ra12,Rb4,X1,Z30), (Ra12,Rb4,X1,Z31), (Ra12,Rb4,X1,Z32), (Ra12,Rb4,X1,Z33), (Ra12,Rb4,X1,Z34), (Ra12,Rb4,X1,Z35), (Ra12,Rb4,X1,Z36), (Ra12,Rb4,X1,Z37), (Ra12,Rb4,X1,Z38), (Ra12,Rb4,X1,Z39), (Ra12,Rb4,X2,Z1), (Ra12,Rb4,X2,Z2), (Ra12,Rb4,X2,Z3), (Ra12,Rb4,X2,Z4), (Ra12,Rb4,X2,Z5), (Ra12,Rb4,X2,Z6), (Ra12,Rb4,X2,Z7), (Ra12,Rb4,X2,Z8), (Ra12,Rb4,X2,Z9), (Ra12,Rb4,X2,Z10), (Ra12,Rb4,X2,Z11), (Ra12,Rb4,X2,Z12), (Ra12,Rb4,X2,Z13), (Ra12,Rb4,X2,Z14), (Ra12,Rb4,X2,Z15), (Ra12,Rb4,X2,Z16), (Ra12,Rb4,X2,Z17), (Ra12,Rb4,X2,Z18), (Ra12,Rb4,X2,Z19), (Ra12,Rb4,X2,Z20), (Ra12,Rb4,X2,Z21), (Ra12,Rb4,X2,Z22), (Ra12,Rb4,X2,Z23), (Ra12,Rb4,X2,Z24), (Ra12,Rb4,X2,Z25), (Ra12,Rb4,X2,Z26), (Ra12,Rb4,X2,Z27), (Ra12,Rb4,X2,Z28), (Ra12,Rb4,X2,Z29), (Ra12,Rb4,X2,Z30), (Ra12,Rb4,X2,Z31), (Ra12,Rb4,X2,Z32), (Ra12,Rb4,X2,Z33), (Ra12,Rb4,X2,Z34), (Ra12,Rb4,X2,Z35), (Ra12,Rb4,X2,Z36), (Ra12,Rb4,X2,Z37), (Ra12,Rb4,X2,Z38), (Ra12,Rb4,X2,Z39), (Ra12,Rb5,X1,Z1), (Ra12,Rb5,X1,Z2), (Ra12,Rb5,X1,Z3), (Ra12,Rb5,X1,Z4), (Ra12,Rb5,X1,Z5), (Ra12,Rb5,X1,Z6), (Ra12,Rb5,X1,Z7), (Ra12,Rb5,X1,Z8), (Ra12,Rb5,X1,Z9), (Ra12,Rb5,X1,Z10), (Ra12,Rb5,X1,Z11), (Ra12,Rb5,X1,Z12), (Ra12,Rb5,X1,Z13), (Ra12,Rb5,X1,Z14), (Ra12,Rb5,X1,Z15), (Ra12,Rb5,X1,Z16), (Ra12,Rb5,X1,Z17), (Ra12,Rb5,X1,Z18), (Ra12,Rb5,X1,Z19), (Ra12,Rb5,X1,Z20), (Ra12,Rb5,X1,Z21), (Ra12,Rb5,X1,Z22), (Ra12,Rb5,X1,Z23), (Ra12,Rb5,X1,Z24), (Ra12,Rb5,X1,Z25), (Ra12,Rb5,X1,Z26), (Ra12,Rb5,X1,Z27), (Ra12,Rb5,X1,Z28), (Ra12,Rb5,X1,Z29), (Ra12,Rb5,X1,Z30), (Ra12,Rb5,X1,Z31), (Ra12,Rb5,X1,Z32), (Ra12,Rb5,X1,Z33), (Ra12,Rb5,X1,Z34), (Ra12,Rb5,X1,Z35), (Ra12,Rb5,X1,Z36), (Ra12,Rb5,X1,Z37), (Ra12,Rb5,X1,Z38), (Ra12,Rb5,X1,Z39), (Ra12,Rb5,X2,Z1), (Ra12,Rb5,X2,Z2), (Ra12,Rb5,X2,Z3), (Ra12,Rb5,X2,Z4), (Ra12,Rb5,X2,Z5), (Ra12,Rb5,X2,Z6), (Ra12,Rb5,X2,Z7), (Ra12,Rb5,X2,Z8), (Ra12,Rb5,X2,Z9), (Ra12,Rb5,X2,Z10), (Ra12,Rb5,X2,Z11), (Ra12,Rb5,X2,Z12), (Ra12,Rb5,X2,Z13), (Ra12,Rb5,X2,Z14), (Ra12,Rb5,X2,Z15), (Ra12,Rb5,X2,Z16), (Ra12,Rb5,X2,Z17), (Ra12,Rb5,X2,Z18), (Ra12,Rb5,X2,Z19), (Ra12,Rb5,X2,Z20), (Ra12,Rb5,X2,Z21), (Ra12,Rb5,X2,Z22), (Ra12,Rb5,X2,Z23), (Ra12,Rb5,X2,Z24), (Ra12,Rb5,X2,Z25), (Ra12,Rb5,X2,Z26), (Ra12,Rb5,X2,Z27), (Ra12,Rb5,X2,Z28), (Ra12,Rb5,X2,Z29), (Ra12,Rb5,X2,Z30), (Ra12,Rb5,X2,Z31), (Ra12,Rb5,X2,Z32), (Ra12,Rb5,X2,Z33), (Ra12,Rb5,X2,Z34), (Ra12,Rb5,X2,Z35), (Ra12,Rb5,X2,Z36), (Ra12,Rb5,X2,Z37), (Ra12,Rb5,X2,Z38), (Ra12,Rb5,X2,Z39), (Ra12,Rb6,X1,Z1), (Ra12,Rb6,X1,Z2), (Ra12,Rb6,X1,Z3), (Ra12,Rb6,X1,Z4), (Ra12,Rb6,X1,Z5), (Ra12,Rb6,X1,Z6), (Ra12,Rb6,X1,Z7), (Ra12,Rb6,X1,Z8), (Ra12,Rb6,X1,Z9), (Ra12,Rb6,X1,Z10), (Ra12,Rb6,X1,Z11), (Ra12,Rb6,X1,Z12), (Ra12,Rb6,X1,Z13), (Ra12,Rb6,X1,Z14), (Ra12,Rb6,X1,Z15), (Ra12,Rb6,X1,Z16), (Ra12,Rb6,X1,Z17), (Ra12,Rb6,X1,Z18), (Ra12,Rb6,X1,Z19), (Ra12,Rb6,X1,Z20), (Ra12,Rb6,X1,Z21), (Ra12,Rb6,X1,Z22), (Ra12,Rb6,X1,Z23), (Ra12,Rb6,X1,Z24), (Ra12,Rb6,X1,Z25), (Ra12,Rb6,X1,Z26), (Ra12,Rb6,X1,Z27), (Ra12,Rb6,X1,Z28), (Ra12,Rb6,X1,Z29), (Ra12,Rb6,X1,Z30), (Ra12,Rb6,X1,Z31), (Ra12,Rb6,X1,Z32), (Ra12,Rb6,X1,Z33), (Ra12,Rb6,X1,Z34), (Ra12,Rb6,X1,Z35), (Ra12,Rb6,X1,Z36), (Ra12,Rb6,X1,Z37), (Ra12,Rb6,X1,Z38), (Ra12,Rb6,X1,Z39), (Ra12,Rb6,X2,Z1), (Ra12,Rb6,X2,Z2), (Ra12,Rb6,X2,Z3), (Ra12,Rb6,X2,Z4), (Ra12,Rb6,X2,Z5), (Ra12,Rb6,X2,Z6), (Ra12,Rb6,X2,Z7), (Ra12,Rb6,X2,Z8), (Ra12,Rb6,X2,Z9), (Ra12,Rb6,X2,Z10), (Ra12,Rb6,X2,Z11), (Ra12,Rb6,X2,Z12), (Ra12,Rb6,X2,Z13), (Ra12,Rb6,X2,Z14), (Ra12,Rb6,X2,Z15), (Ra12,Rb6,X2,Z16), (Ra12,Rb6,X2,Z17), (Ra12,Rb6,X2,Z18), (Ra12,Rb6,X2,Z19), (Ra12,Rb6,X2,Z20), (Ra12,Rb6,X2,Z21), (Ra12,Rb6,X2,Z22), (Ra12,Rb6,X2,Z23), (Ra12,Rb6,X2,Z24), (Ra12,Rb6,X2,Z25), (Ra12,Rb6,X2,Z26), (Ra12,Rb6,X2,Z27), (Ra12,Rb6,X2,Z28), (Ra12,Rb6,X2,Z29), (Ra12,Rb6,X2,Z30), (Ra12,Rb6,X2,Z31), (Ra12,Rb6,X2,Z32), (Ra12,Rb6,X2,Z33), (Ra12,Rb6,X2,Z34), (Ra12,Rb6,X2,Z35), (Ra12,Rb6,X2,Z36), (Ra12,Rb6,X2,Z37), (Ra12,Rb6,X2,Z38), (Ra12,Rb6,X2,Z39), (Ra12,Rb7,X1,Z1), (Ra12,Rb7,X1,Z2), (Ra12,Rb7,X1,Z3), (Ra12,Rb7,X1,Z4), (Ra12,Rb7,X1,Z5), (Ra12,Rb7,X1,Z6), (Ra12,Rb7,X1,Z7), (Ra12,Rb7,X1,Z8), (Ra12,Rb7,X1,Z9), (Ra12,Rb7,X1,Z10), (Ra12,Rb7,X1,Z11), (Ra12,Rb7,X1,Z12), (Ra12,Rb7,X1,Z13), (Ra12,Rb7,X1,Z14), (Ra12,Rb7,X1,Z15), (Ra12,Rb7,X1,Z16), (Ra12,Rb7,X1,Z17), (Ra12,Rb7,X1,Z18), (Ra12,Rb7,X1,Z19), (Ra12,Rb7,X1,Z20), (Ra12,Rb7,X1,Z21), (Ra12,Rb7,X1,Z22), (Ra12,Rb7,X1,Z23), (Ra12,Rb7,X1,Z24), (Ra12,Rb7,X1,Z25), (Ra12,Rb7,X1,Z26), (Ra12,Rb7,X1,Z27), (Ra12,Rb7,X1,Z28), (Ra12,Rb7,X1,Z29), (Ra12,Rb7,X1,Z30), (Ra12,Rb7,X1,Z31), (Ra12,Rb7,X1,Z32), (Ra12,Rb7,X1,Z33), (Ra12,Rb7,X1,Z34), (Ra12,Rb7,X1,Z35), (Ra12,Rb7,X1,Z36), (Ra12,Rb7,X1,Z37), (Ra12,Rb7,X1,Z38), (Ra12,Rb7,X1,Z39), (Ra12,Rb7,X2,Z1), (Ra12,Rb7,X2,Z2), (Ra12,Rb7,X2,Z3), (Ra12,Rb7,X2,Z4), (Ra12,Rb7,X2,Z5), (Ra12,Rb7,X2,Z6), (Ra12,Rb7,X2,Z7), (Ra12,Rb7,X2,Z8), (Ra12,Rb7,X2,Z9), (Ra12,Rb7,X2,Z10), (Ra12,Rb7,X2,Z11), (Ra12,Rb7,X2,Z12), (Ra12,Rb7,X2,Z13), (Ra12,Rb7,X2,Z14), (Ra12,Rb7,X2,Z15), (Ra12,Rb7,X2,Z16), (Ra12,Rb7,X2,Z17), (Ra12,Rb7,X2,Z18), (Ra12,Rb7,X2,Z19), (Ra12,Rb7,X2,Z20), (Ra12,Rb7,X2,Z21), (Ra12,Rb7,X2,Z22), (Ra12,Rb7,X2,Z23), (Ra12,Rb7,X2,Z24), (Ra12,Rb7,X2,Z25), (Ra12,Rb7,X2,Z26), (Ra12,Rb7,X2,Z27), (Ra12,Rb7,X2,Z28), (Ra12,Rb7,X2,Z29), (Ra12,Rb7,X2,Z30), (Ra12,Rb7,X2,Z31), (Ra12,Rb7,X2,Z32), (Ra12,Rb7,X2,Z33), (Ra12,Rb7,X2,Z34), (Ra12,Rb7,X2,Z35), (Ra12,Rb7,X2,Z36), (Ra12,Rb7,X2,Z37), (Ra12,Rb7,X2,Z38), (Ra12,Rb7,X2,Z39), (Ra12,Rb8,X1,Z1), (Ra12,Rb8,X1,Z2), (Ra12,Rb8,X1,Z3), (Ra12,Rb8,X1,Z4), (Ra12,Rb8,X1,Z5), (Ra12,Rb8,X1,Z6), (Ra12,Rb8,X1,Z7), (Ra12,Rb8,X1,Z8), (Ra12,Rb8,X1,Z9), (Ra12,Rb8,X1,Z10), (Ra12,Rb8,X1,Z11), (Ra12,Rb8,X1,Z12), (Ra12,Rb8,X1,Z13), (Ra12,Rb8,X1,Z14), (Ra12,Rb8,X1,Z15), (Ra12,Rb8,X1,Z16), (Ra12,Rb8,X1,Z17), (Ra12,Rb8,X1,Z18), (Ra12,Rb8,X1,Z19), (Ra12,Rb8,X1,Z20), (Ra12,Rb8,X1,Z21), (Ra12,Rb8,X1,Z22), (Ra12,Rb8,X1,Z23), (Ra12,Rb8,X1,Z24), (Ra12,Rb8,X1,Z25), (Ra12,Rb8,X1,Z26), (Ra12,Rb8,X1,Z27), (Ra12,Rb8,X1,Z28), (Ra12,Rb8,X1,Z29), (Ra12,Rb8,X1,Z30), (Ra12,Rb8,X1,Z31), (Ra12,Rb8,X1,Z32), (Ra12,Rb8,X1,Z33), (Ra12,Rb8,X1,Z34), (Ra12,Rb8,X1,Z35), (Ra12,Rb8,X1,Z36), (Ra12,Rb8,X1,Z37), (Ra12,Rb8,X1,Z38), (Ra12,Rb8,X1,Z39), (Ra12,Rb8,X2,Z1), (Ra12,Rb8,X2,Z2), (Ra12,Rb8,X2,Z3), (Ra12,Rb8,X2,Z4), (Ra12,Rb8,X2,Z5), (Ra12,Rb8,X2,Z6), (Ra12,Rb8,X2,Z7), (Ra12,Rb8,X2,Z8), (Ra12,Rb8,X2,Z9), (Ra12,Rb8,X2,Z10), (Ra12,Rb8,X2,Z11), (Ra12,Rb8,X2,Z12), (Ra12,Rb8,X2,Z13), (Ra12,Rb8,X2,Z14), (Ra12,Rb8,X2,Z15), (Ra12,Rb8,X2,Z16), (Ra12,Rb8,X2,Z17), (Ra12,Rb8,X2,Z18), (Ra12,Rb8,X2,Z19), (Ra12,Rb8,X2,Z20), (Ra12,Rb8,X2,Z21), (Ra12,Rb8,X2,Z22), (Ra12,Rb8,X2,Z23), (Ra12,Rb8,X2,Z24), (Ra12,Rb8,X2,Z25), (Ra12,Rb8,X2,Z26), (Ra12,Rb8,X2,Z27), (Ra12,Rb8,X2,Z28), (Ra12,Rb8,X2,Z29), (Ra12,Rb8,X2,Z30), (Ra12,Rb8,X2,Z31), (Ra12,Rb8,X2,Z32), (Ra12,Rb8,X2,Z33), (Ra12,Rb8,X2,Z34), (Ra12,Rb8,X2,Z35), (Ra12,Rb8,X2,Z36), (Ra12,Rb8,X2,Z37), (Ra12,Rb8,X2,Z38), (Ra12,Rb8,X2,Z39), (Ra13,Rb1,X1,Z1), (Ra13,Rb1,X1,Z2), (Ra13,Rb1,X1,Z3), (Ra13,Rb1,X1,Z4), (Ra13,Rb1,X1,Z5), (Ra13,Rb1,X1,Z6), (Ra13,Rb1,X1,Z7), (Ra13,Rb1,X1,Z8), (Ra13,Rb1,X1,Z9), (Ra13,Rb1,X1,Z10), (Ra13,Rb1,X1,Z11), (Ra13,Rb1,X1,Z12), (Ra13,Rb1,X1,Z13), (Ra13,Rb1,X1,Z14), (Ra13,Rb1,X1,Z15), (Ra13,Rb1,X1,Z16), (Ra13,Rb1,X1,Z17), (Ra13,Rb1,X1,Z18), (Ra13,Rb1,X1,Z19), (Ra13,Rb1,X1,Z20), (Ra13,Rb1,X1,Z21), (Ra13,Rb1,X1,Z22), (Ra13,Rb1,X1,Z23), (Ra13,Rb1,X1,Z24), (Ra13,Rb1,X1,Z25), (Ra13,Rb1,X1,Z26), (Ra13,Rb1,X1,Z27), (Ra13,Rb1,X1,Z28), (Ra13,Rb1,X1,Z29), (Ra13,Rb1,X1,Z30), (Ra13,Rb1,X1,Z31), (Ra13,Rb1,X1,Z32), (Ra13,Rb1,X1,Z33), (Ra13,Rb1,X1,Z34), (Ra13,Rb1,X1,Z35), (Ra13,Rb1,X1,Z36), (Ra13,Rb1,X1,Z37), (Ra13,Rb1,X1,Z38), (Ra13,Rb1,X1,Z39), (Ra13,Rb1,X2,Z1), (Ra13,Rb1,X2,Z2), (Ra13,Rb1,X2,Z3), (Ra13,Rb1,X2,Z4), (Ra13,Rb1,X2,Z5), (Ra13,Rb1,X2,Z6), (Ra13,Rb1,X2,Z7), (Ra13,Rb1,X2,Z8), (Ra13,Rb1,X2,Z9), (Ra13,Rb1,X2,Z10), (Ra13,Rb1,X2,Z11), (Ra13,Rb1,X2,Z12), (Ra13,Rb1,X2,Z13), (Ra13,Rb1,X2,Z14), (Ra13,Rb1,X2,Z15), (Ra13,Rb1,X2,Z16), (Ra13,Rb1,X2,Z17), (Ra13,Rb1,X2,Z18), (Ra13,Rb1,X2,Z19), (Ra13,Rb1,X2,Z20), (Ra13,Rb1,X2,Z21), (Ra13,Rb1,X2,Z22), (Ra13,Rb1,X2,Z23), (Ra13,Rb1,X2,Z24), (Ra13,Rb1,X2,Z25), (Ra13,Rb1,X2,Z26), (Ra13,Rb1,X2,Z27), (Ra13,Rb1,X2,Z28), (Ra13,Rb1,X2,Z29), (Ra13,Rb1,X2,Z30), (Ra13,Rb1,X2,Z31), (Ra13,Rb1,X2,Z32), (Ra13,Rb1,X2,Z33), (Ra13,Rb1,X2,Z34), (Ra13,Rb1,X2,Z35), (Ra13,Rb1,X2,Z36), (Ra13,Rb1,X2,Z37), (Ra13,Rb1,X2,Z38), (Ra13,Rb1,X2,Z39), (Ra13,Rb2,X1,Z1), (Ra13,Rb2,X1,Z2), (Ra13,Rb2,X1,Z3), (Ra13,Rb2,X1,Z4), (Ra13,Rb2,X1,Z5), (Ra13,Rb2,X1,Z6), (Ra13,Rb2,X1,Z7), (Ra13,Rb2,X1,Z8), (Ra13,Rb2,X1,Z9), (Ra13,Rb2,X1,Z10), (Ra13,Rb2,X1,Z11), (Ra13,Rb2,X1,Z12), (Ra13,Rb2,X1,Z13), (Ra13,Rb2,X1,Z14), (Ra13,Rb2,X1,Z15), (Ra13,Rb2,X1,Z16), (Ra13,Rb2,X1,Z17), (Ra13,Rb2,X1,Z18), (Ra13,Rb2,X1,Z19), (Ra13,Rb2,X1,Z20), (Ra13,Rb2,X1,Z21), (Ra13,Rb2,X1,Z22), (Ra13,Rb2,X1,Z23), (Ra13,Rb2,X1,Z24), (Ra13,Rb2,X1,Z25), (Ra13,Rb2,X1,Z26), (Ra13,Rb2,X1,Z27), (Ra13,Rb2,X1,Z28), (Ra13,Rb2,X1,Z29), (Ra13,Rb2,X1,Z30), (Ra13,Rb2,X1,Z31), (Ra13,Rb2,X1,Z32), (Ra13,Rb2,X1,Z33), (Ra13,Rb2,X1,Z34), (Ra13,Rb2,X1,Z35), (Ra13,Rb2,X1,Z36), (Ra13,Rb2,X1,Z37), (Ra13,Rb2,X1,Z38), (Ra13,Rb2,X1,Z39), (Ra13,Rb2,X2,Z1), (Ra13,Rb2,X2,Z2), (Ra13,Rb2,X2,Z3), (Ra13,Rb2,X2,Z4), (Ra13,Rb2,X2,Z5), (Ra13,Rb2,X2,Z6), (Ra13,Rb2,X2,Z7), (Ra13,Rb2,X2,Z8), (Ra13,Rb2,X2,Z9), (Ra13,Rb2,X2,Z10), (Ra13,Rb2,X2,Z11), (Ra13,Rb2,X2,Z12), (Ra13,Rb2,X2,Z13), (Ra13,Rb2,X2,Z14), (Ra13,Rb2,X2,Z15), (Ra13,Rb2,X2,Z16), (Ra13,Rb2,X2,Z17), (Ra13,Rb2,X2,Z18), (Ra13,Rb2,X2,Z19), (Ra13,Rb2,X2,Z20), (Ra13,Rb2,X2,Z21), (Ra13,Rb2,X2,Z22), (Ra13,Rb2,X2,Z23), (Ra13,Rb2,X2,Z24), (Ra13,Rb2,X2,Z25), (Ra13,Rb2,X2,Z26), (Ra13,Rb2,X2,Z27), (Ra13,Rb2,X2,Z28), (Ra13,Rb2,X2,Z29), (Ra13,Rb2,X2,Z30), (Ra13,Rb2,X2,Z31), (Ra13,Rb2,X2,Z32), (Ra13,Rb2,X2,Z33), (Ra13,Rb2,X2,Z34), (Ra13,Rb2,X2,Z35), (Ra13,Rb2,X2,Z36), (Ra13,Rb2,X2,Z37), (Ra13,Rb2,X2,Z38), (Ra13,Rb2,X2,Z39), (Ra13,Rb3,X1,Z1), (Ra13,Rb3,X1,Z2), (Ra13,Rb3,X1,Z3), (Ra13,Rb3,X1,Z4), (Ra13,Rb3,X1,Z5), (Ra13,Rb3,X1,Z6), (Ra13,Rb3,X1,Z7), (Ra13,Rb3,X1,Z8), (Ra13,Rb3,X1,Z9), (Ra13,Rb3,X1,Z10), (Ra13,Rb3,X1,Z11), (Ra13,Rb3,X1,Z12), (Ra13,Rb3,X1,Z13), (Ra13,Rb3,X1,Z14), (Ra13,Rb3,X1,Z15), (Ra13,Rb3,X1,Z16), (Ra13,Rb3,X1,Z17), (Ra13,Rb3,X1,Z18), (Ra13,Rb3,X1,Z19), (Ra13,Rb3,X1,Z20), (Ra13,Rb3,X1,Z21), (Ra13,Rb3,X1,Z22), (Ra13,Rb3,X1,Z23), (Ra13,Rb3,X1,Z24), (Ra13,Rb3,X1,Z25), (Ra13,Rb3,X1,Z26), (Ra13,Rb3,X1,Z27), (Ra13,Rb3,X1,Z28), (Ra13,Rb3,X1,Z29), (Ra13,Rb3,X1,Z30), (Ra13,Rb3,X1,Z31), (Ra13,Rb3,X1,Z32), (Ra13,Rb3,X1,Z33), (Ra13,Rb3,X1,Z34), (Ra13,Rb3,X1,Z35), (Ra13,Rb3,X1,Z36), (Ra13,Rb3,X1,Z37), (Ra13,Rb3,X1,Z38), (Ra13,Rb3,X1,Z39), (Ra13,Rb3,X2,Z1), (Ra13,Rb3,X2,Z2), (Ra13,Rb3,X2,Z3), (Ra13,Rb3,X2,Z4), (Ra13,Rb3,X2,Z5), (Ra13,Rb3,X2,Z6), (Ra13,Rb3,X2,Z7), (Ra13,Rb3,X2,Z8), (Ra13,Rb3,X2,Z9), (Ra13,Rb3,X2,Z10), (Ra13,Rb3,X2,Z11), (Ra13,Rb3,X2,Z12), (Ra13,Rb3,X2,Z13), (Ra13,Rb3,X2,Z14), (Ra13,Rb3,X2,Z15), (Ra13,Rb3,X2,Z16), (Ra13,Rb3,X2,Z17), (Ra13,Rb3,X2,Z18), (Ra13,Rb3,X2,Z19), (Ra13,Rb3,X2,Z20), (Ra13,Rb3,X2,Z21), (Ra13,Rb3,X2,Z22), (Ra13,Rb3,X2,Z23), (Ra13,Rb3,X2,Z24), (Ra13,Rb3,X2,Z25), (Ra13,Rb3,X2,Z26), (Ra13,Rb3,X2,Z27), (Ra13,Rb3,X2,Z28), (Ra13,Rb3,X2,Z29), (Ra13,Rb3,X2,Z30), (Ra13,Rb3,X2,Z31), (Ra13,Rb3,X2,Z32), (Ra13,Rb3,X2,Z33), (Ra13,Rb3,X2,Z34), (Ra13,Rb3,X2,Z35), (Ra13,Rb3,X2,Z36), (Ra13,Rb3,X2,Z37), (Ra13,Rb3,X2,Z38), (Ra13,Rb3,X2,Z39), (Ra13,Rb4,X1,Z1), (Ra13,Rb4,X1,Z2), (Ra13,Rb4,X1,Z3), (Ra13,Rb4,X1,Z4), (Ra13,Rb4,X1,Z5), (Ra13,Rb4,X1,Z6), (Ra13,Rb4,X1,Z7), (Ra13,Rb4,X1,Z8), (Ra13,Rb4,X1,Z9), (Ra13,Rb4,X1,Z10), (Ra13,Rb4,X1,Z11), (Ra13,Rb4,X1,Z12), (Ra13,Rb4,X1,Z13), (Ra13,Rb4,X1,Z14), (Ra13,Rb4,X1,Z15), (Ra13,Rb4,X1,Z16), (Ra13,Rb4,X1,Z17), (Ra13,Rb4,X1,Z18), (Ra13,Rb4,X1,Z19), (Ra13,Rb4,X1,Z20), (Ra13,Rb4,X1,Z21), (Ra13,Rb4,X1,Z22), (Ra13,Rb4,X1,Z23), (Ra13,Rb4,X1,Z24), (Ra13,Rb4,X1,Z25), (Ra13,Rb4,X1,Z26), (Ra13,Rb4,X1,Z27), (Ra13,Rb4,X1,Z28), (Ra13,Rb4,X1,Z29), (Ra13,Rb4,X1,Z30), (Ra13,Rb4,X1,Z31), (Ra13,Rb4,X1,Z32), (Ra13,Rb4,X1,Z33), (Ra13,Rb4,X1,Z34), (Ra13,Rb4,X1,Z35), (Ra13,Rb4,X1,Z36), (Ra13,Rb4,X1,Z37), (Ra13,Rb4,X1,Z38), (Ra13,Rb4,X1,Z39), (Ra13,Rb4,X2,Z1), (Ra13,Rb4,X2,Z2), (Ra13,Rb4,X2,Z3), (Ra13,Rb4,X2,Z4), (Ra13,Rb4,X2,Z5), (Ra13,Rb4,X2,Z6), (Ra13,Rb4,X2,Z7), (Ra13,Rb4,X2,Z8), (Ra13,Rb4,X2,Z9), (Ra13,Rb4,X2,Z10), (Ra13,Rb4,X2,Z11), (Ra13,Rb4,X2,Z12), (Ra13,Rb4,X2,Z13), (Ra13,Rb4,X2,Z14), (Ra13,Rb4,X2,Z15), (Ra13,Rb4,X2,Z16), (Ra13,Rb4,X2,Z17), (Ra13,Rb4,X2,Z18), (Ra13,Rb4,X2,Z19), (Ra13,Rb4,X2,Z20), (Ra13,Rb4,X2,Z21), (Ra13,Rb4,X2,Z22), (Ra13,Rb4,X2,Z23), (Ra13,Rb4,X2,Z24), (Ra13,Rb4,X2,Z25), (Ra13,Rb4,X2,Z26), (Ra13,Rb4,X2,Z27), (Ra13,Rb4,X2,Z28), (Ra13,Rb4,X2,Z29), (Ra13,Rb4,X2,Z30), (Ra13,Rb4,X2,Z31), (Ra13,Rb4,X2,Z32), (Ra13,Rb4,X2,Z33), (Ra13,Rb4,X2,Z34), (Ra13,Rb4,X2,Z35), (Ra13,Rb4,X2,Z36), (Ra13,Rb4,X2,Z37), (Ra13,Rb4,X2,Z38), (Ra13,Rb4,X2,Z39), (Ra13,Rb5,X1,Z1), (Ra13,Rb5,X1,Z2), (Ra13,Rb5,X1,Z3), (Ra13,Rb5,X1,Z4), (Ra13,Rb5,X1,Z5), (Ra13,Rb5,X1,Z6), (Ra13,Rb5,X1,Z7), (Ra13,Rb5,X1,Z8), (Ra13,Rb5,X1,Z9), (Ra13,Rb5,X1,Z10), (Ra13,Rb5,X1,Z11), (Ra13,Rb5,X1,Z12), (Ra13,Rb5,X1,Z13), (Ra13,Rb5,X1,Z14), (Ra13,Rb5,X1,Z15), (Ra13,Rb5,X1,Z16), (Ra13,Rb5,X1,Z17), (Ra13,Rb5,X1,Z18), (Ra13,Rb5,X1,Z19), (Ra13,Rb5,X1,Z20), (Ra13,Rb5,X1,Z21), (Ra13,Rb5,X1,Z22), (Ra13,Rb5,X1,Z23), (Ra13,Rb5,X1,Z24), (Ra13,Rb5,X1,Z25), (Ra13,Rb5,X1,Z26), (Ra13,Rb5,X1,Z27), (Ra13,Rb5,X1,Z28), (Ra13,Rb5,X1,Z29), (Ra13,Rb5,X1,Z30), (Ra13,Rb5,X1,Z31), (Ra13,Rb5,X1,Z32), (Ra13,Rb5,X1,Z33), (Ra13,Rb5,X1,Z34), (Ra13,Rb5,X1,Z35), (Ra13,Rb5,X1,Z36), (Ra13,Rb5,X1,Z37), (Ra13,Rb5,X1,Z38), (Ra13,Rb5,X1,Z39), (Ra13,Rb5,X2,Z1), (Ra13,Rb5,X2,Z2), (Ra13,Rb5,X2,Z3), (Ra13,Rb5,X2,Z4), (Ra13,Rb5,X2,Z5), (Ra13,Rb5,X2,Z6), (Ra13,Rb5,X2,Z7), (Ra13,Rb5,X2,Z8), (Ra13,Rb5,X2,Z9), (Ra13,Rb5,X2,Z10), (Ra13,Rb5,X2,Z11), (Ra13,Rb5,X2,Z12), (Ra13,Rb5,X2,Z13), (Ra13,Rb5,X2,Z14), (Ra13,Rb5,X2,Z15), (Ra13,Rb5,X2,Z16), (Ra13,Rb5,X2,Z17), (Ra13,Rb5,X2,Z18), (Ra13,Rb5,X2,Z19), (Ra13,Rb5,X2,Z20), (Ra13,Rb5,X2,Z21), (Ra13,Rb5,X2,Z22), (Ra13,Rb5,X2,Z23), (Ra13,Rb5,X2,Z24), (Ra13,Rb5,X2,Z25), (Ra13,Rb5,X2,Z26), (Ra13,Rb5,X2,Z27), (Ra13,Rb5,X2,Z28), (Ra13,Rb5,X2,Z29), (Ra13,Rb5,X2,Z30), (Ra13,Rb5,X2,Z31), (Ra13,Rb5,X2,Z32), (Ra13,Rb5,X2,Z33), (Ra13,Rb5,X2,Z34), (Ra13,Rb5,X2,Z35), (Ra13,Rb5,X2,Z36), (Ra13,Rb5,X2,Z37), (Ra13,Rb5,X2,Z38), (Ra13,Rb5,X2,Z39), (Ra13,Rb6,X1,Z1), 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(Ra15,Rb2,X1,Z20), (Ra15,Rb2,X1,Z21), (Ra15,Rb2,X1,Z22), (Ra15,Rb2,X1,Z23), (Ra15,Rb2,X1,Z24), (Ra15,Rb2,X1,Z25), (Ra15,Rb2,X1,Z26), (Ra15,Rb2,X1,Z27), (Ra15,Rb2,X1,Z28), (Ra15,Rb2,X1,Z29), (Ra15,Rb2,X1,Z30), (Ra15,Rb2,X1,Z31), (Ra15,Rb2,X1,Z32), (Ra15,Rb2,X1,Z33), (Ra15,Rb2,X1,Z34), (Ra15,Rb2,X1,Z35), (Ra15,Rb2,X1,Z36), (Ra15,Rb2,X1,Z37), (Ra15,Rb2,X1,Z38), (Ra15,Rb2,X1,Z39), (Ra15,Rb2,X2,Z1), (Ra15,Rb2,X2,Z2), (Ra15,Rb2,X2,Z3), (Ra15,Rb2,X2,Z4), (Ra15,Rb2,X2,Z5), (Ra15,Rb2,X2,Z6), (Ra15,Rb2,X2,Z7), (Ra15,Rb2,X2,Z8), (Ra15,Rb2,X2,Z9), (Ra15,Rb2,X2,Z10), (Ra15,Rb2,X2,Z11), (Ra15,Rb2,X2,Z12), (Ra15,Rb2,X2,Z13), (Ra15,Rb2,X2,Z14), (Ra15,Rb2,X2,Z15), (Ra15,Rb2,X2,Z16), (Ra15,Rb2,X2,Z17), (Ra15,Rb2,X2,Z18), (Ra15,Rb2,X2,Z19), (Ra15,Rb2,X2,Z20), (Ra15,Rb2,X2,Z21), (Ra15,Rb2,X2,Z22), (Ra15,Rb2,X2,Z23), (Ra15,Rb2,X2,Z24), (Ra15,Rb2,X2,Z25), (Ra15,Rb2,X2,Z26), (Ra15,Rb2,X2,Z27), (Ra15,Rb2,X2,Z28), (Ra15,Rb2,X2,Z29), (Ra15,Rb2,X2,Z30), (Ra15,Rb2,X2,Z31), (Ra15,Rb2,X2,Z32), (Ra15,Rb2,X2,Z33), (Ra15,Rb2,X2,Z34), (Ra15,Rb2,X2,Z35), (Ra15,Rb2,X2,Z36), (Ra15,Rb2,X2,Z37), (Ra15,Rb2,X2,Z38), (Ra15,Rb2,X2,Z39), (Ra15,Rb3,X1,Z1), (Ra15,Rb3,X1,Z2), (Ra15,Rb3,X1,Z3), (Ra15,Rb3,X1,Z4), (Ra15,Rb3,X1,Z5), (Ra15,Rb3,X1,Z6), (Ra15,Rb3,X1,Z7), (Ra15,Rb3,X1,Z8), (Ra15,Rb3,X1,Z9), (Ra15,Rb3,X1,Z10), (Ra15,Rb3,X1,Z11), (Ra15,Rb3,X1,Z12), (Ra15,Rb3,X1,Z13), (Ra15,Rb3,X1,Z14), (Ra15,Rb3,X1,Z15), (Ra15,Rb3,X1,Z16), (Ra15,Rb3,X1,Z17), (Ra15,Rb3,X1,Z18), (Ra15,Rb3,X1,Z19), (Ra15,Rb3,X1,Z20), (Ra15,Rb3,X1,Z21), (Ra15,Rb3,X1,Z22), (Ra15,Rb3,X1,Z23), (Ra15,Rb3,X1,Z24), (Ra15,Rb3,X1,Z25), (Ra15,Rb3,X1,Z26), (Ra15,Rb3,X1,Z27), (Ra15,Rb3,X1,Z28), (Ra15,Rb3,X1,Z29), (Ra15,Rb3,X1,Z30), (Ra15,Rb3,X1,Z31), (Ra15,Rb3,X1,Z32), (Ra15,Rb3,X1,Z33), (Ra15,Rb3,X1,Z34), (Ra15,Rb3,X1,Z35), (Ra15,Rb3,X1,Z36), (Ra15,Rb3,X1,Z37), (Ra15,Rb3,X1,Z38), (Ra15,Rb3,X1,Z39), (Ra15,Rb3,X2,Z1), (Ra15,Rb3,X2,Z2), (Ra15,Rb3,X2,Z3), (Ra15,Rb3,X2,Z4), (Ra15,Rb3,X2,Z5), (Ra15,Rb3,X2,Z6), (Ra15,Rb3,X2,Z7), (Ra15,Rb3,X2,Z8), (Ra15,Rb3,X2,Z9), (Ra15,Rb3,X2,Z10), (Ra15,Rb3,X2,Z11), (Ra15,Rb3,X2,Z12), (Ra15,Rb3,X2,Z13), (Ra15,Rb3,X2,Z14), (Ra15,Rb3,X2,Z15), (Ra15,Rb3,X2,Z16), (Ra15,Rb3,X2,Z17), (Ra15,Rb3,X2, Z18), (Ra15,Rb3,X2,Z19), (Ra15,Rb3,X2,Z20), (Ra15,Rb3,X2,Z21), (Ra15,Rb3,X2,Z22), (Ra15,Rb3,X2,Z23), (Ra15,Rb3,X2,Z24), (Ra15,Rb3,X2,Z25), (Ra15,Rb3,X2,Z26), (Ra15,Rb3,X2,Z27), (Ra15,Rb3,X2,Z28), (Ra15,Rb3,X2,Z29), (Ra15,Rb3,X2,Z30), (Ra15,Rb3,X2,Z31), (Ra15,Rb3,X2,Z32), (Ra15,Rb3,X2,Z33), (Ra15,Rb3,X2,Z34), (Ra15,Rb3,X2,Z35), (Ra15,Rb3,X2,Z36), (Ra15,Rb3,X2,Z37), (Ra15,Rb3,X2,Z38), (Ra15,Rb3,X2,Z39), (Ra15,Rb4,X1,Z1), (Ra15,Rb4,X1,Z2), (Ra15,Rb4,X1,Z3), (Ra15,Rb4,X1,Z4), (Ra15,Rb4,X1,Z5), (Ra15,Rb4,X1,Z6), (Ra15,Rb4,X1,Z7), (Ra15,Rb4,X1,Z8), (Ra15,Rb4,X1,Z9), (Ra15,Rb4,X1,Z10), (Ra15,Rb4,X1,Z11), (Ra15,Rb4,X1,Z12), (Ra15,Rb4,X1,Z13), (Ra15,Rb4,X1,Z14), (Ra15,Rb4,X1,Z15), (Ra15,Rb4,X1,Z16), (Ra15,Rb4,X1,Z17), (Ra15,Rb4,X1,Z18), (Ra15,Rb4,X1,Z19), (Ra15,Rb4,X1,Z20), (Ra15,Rb4,X1,Z21), (Ra15,Rb4,X1,Z22), (Ra15,Rb4,X1,Z23), (Ra15,Rb4,X1,Z24), (Ra15,Rb4,X1,Z25), (Ra15,Rb4,X1,Z26), (Ra15,Rb4,X1,Z27), (Ra15,Rb4,X1,Z28), (Ra15,Rb4,X1,Z29), (Ra15,Rb4,X1,Z30), (Ra15,Rb4,X1,Z31), (Ra15,Rb4,X1,Z32), (Ra15,Rb4,X1,Z33), (Ra15,Rb4,X1,Z34), (Ra15,Rb4,X1,Z35), (Ra15,Rb4,X1,Z36), (Ra15,Rb4,X1,Z37), (Ra15,Rb4,X1,Z38), (Ra15,Rb4,X1,Z39), (Ra15,Rb4,X2,Z1), (Ra15,Rb4,X2,Z2), (Ra15,Rb4,X2,Z3), (Ra15,Rb4,X2,Z4), (Ra15,Rb4,X2,Z5), (Ra15,Rb4,X2,Z6), (Ra15,Rb4,X2,Z7), (Ra15,Rb4,X2,Z8), (Ra15,Rb4,X2,Z9), (Ra15,Rb4,X2,Z10), (Ra15,Rb4,X2,Z11), (Ra15,Rb4,X2,Z12), (Ra15,Rb4,X2,Z13), (Ra15,Rb4,X2,Z14), (Ra15,Rb4,X2,Z15), (Ra15,Rb4,X2,Z16), (Ra15,Rb4,X2,Z17), (Ra15,Rb4,X2,Z18), (Ra15,Rb4,X2,Z19), (Ra15,Rb4,X2,Z20), (Ra15,Rb4,X2,Z21), (Ra15,Rb4,X2,Z22), (Ra15,Rb4,X2,Z23), (Ra15,Rb4,X2,Z24), (Ra15,Rb4,X2,Z25), (Ra15,Rb4,X2,Z26), (Ra15,Rb4,X2,Z27), (Ra15,Rb4,X2,Z28), (Ra15,Rb4,X2,Z29), (Ra15,Rb4,X2,Z30), (Ra15,Rb4,X2,Z31), (Ra15,Rb4,X2,Z32), (Ra15,Rb4,X2,Z33), (Ra15,Rb4,X2,Z34), (Ra15,Rb4,X2,Z35), (Ra15,Rb4,X2,Z36), (Ra15,Rb4,X2,Z37), (Ra15,Rb4,X2,Z38), (Ra15,Rb4,X2,Z39), (Ra15,Rb5,X1,Z1), (Ra15,Rb5,X1,Z2), (Ra15,Rb5,X1,Z3), (Ra15,Rb5,X1,Z4), (Ra15,Rb5,X1,Z5), (Ra15,Rb5,X1,Z6), (Ra15,Rb5,X1,Z7), (Ra15,Rb5,X1,Z8), (Ra15,Rb5,X1,Z9), (Ra15,Rb5,X1,Z10), (Ra15,Rb5,X1,Z11), (Ra15,Rb5,X1,Z12), (Ra15,Rb5,X1,Z13), (Ra15,Rb5,X1,Z14), (Ra15,Rb5,X1,Z15), (Ra15,Rb5,X1,Z16), (Ra15,Rb5,X1,Z17), (Ra15,Rb5,X1,Z18), (Ra15,Rb5,X1,Z19), (Ra15,Rb5,X1,Z20), (Ra15,Rb5,X1,Z21), (Ra15,Rb5,X1,Z22), (Ra15,Rb5,X1,Z23), (Ra15,Rb5,X1,Z24), (Ra15,Rb5,X1,Z25), (Ra15,Rb5,X1,Z26), (Ra15,Rb5,X1,Z27), (Ra15,Rb5,X1,Z28), (Ra15,Rb5,X1,Z29), (Ra15,Rb5,X1,Z30), (Ra15,Rb5,X1,Z31), (Ra15,Rb5,X1,Z32), (Ra15,Rb5,X1,Z33), (Ra15,Rb5,X1,Z34), (Ra15,Rb5,X1,Z35), (Ra15,Rb5,X1,Z36), (Ra15,Rb5,X1,Z37), (Ra15,Rb5,X1,Z38), (Ra15,Rb5,X1,Z39), (Ra15,Rb5,X2,Z1), (Ra15,Rb5,X2,Z2), (Ra15,Rb5,X2,Z3), (Ra15,Rb5,X2,Z4), (Ra15,Rb5,X2,Z5), (Ra15,Rb5,X2,Z6), (Ra15,Rb5,X2,Z7), (Ra15,Rb5,X2,Z8), (Ra15,Rb5,X2,Z9), (Ra15,Rb5,X2,Z10), (Ra15,Rb5,X2,Z11), (Ra15,Rb5,X2,Z12), (Ra15,Rb5,X2,Z13), (Ra15,Rb5,X2,Z14), (Ra15,Rb5,X2,Z15), (Ra15,Rb5,X2,Z16), (Ra15,Rb5,X2,Z17), (Ra15,Rb5,X2,Z18), (Ra15,Rb5,X2,Z19), (Ra15,Rb5,X2,Z20), (Ra15,Rb5,X2,Z21), (Ra15,Rb5,X2,Z22), (Ra15,Rb5,X2,Z23), (Ra15,Rb5,X2,Z24), (Ra15,Rb5,X2,Z25), (Ra15,Rb5,X2,Z26), (Ra15,Rb5,X2,Z27), (Ra15,Rb5,X2,Z28), (Ra15,Rb5,X2,Z29), (Ra15,Rb5,X2,Z30), (Ra15,Rb5,X2,Z31), (Ra15,Rb5,X2,Z32), (Ra15,Rb5,X2,Z33), (Ra15,Rb5,X2,Z34), (Ra15,Rb5,X2,Z35), (Ra15,Rb5,X2,Z36), (Ra15,Rb5,X2,Z37), (Ra15,Rb5,X2,Z38), (Ra15,Rb5,X2,Z39), (Ra15,Rb6,X1,Z1), (Ra15,Rb6,X1,Z2), (Ra15,Rb6,X1,Z3), (Ra15,Rb6,X1,Z4), (Ra15,Rb6,X1,Z5), (Ra15,Rb6,X1,Z6), (Ra15,Rb6,X1,Z7), (Ra15,Rb6,X1,Z8), (Ra15,Rb6,X1,Z9), (Ra15,Rb6,X1,Z10), (Ra15,Rb6,X1,Z11), (Ra15,Rb6,X1,Z12), (Ra15,Rb6,X1,Z13), (Ra15,Rb6,X1,Z14), (Ra15,Rb6,X1,Z15), (Ra15,Rb6,X1,Z16), (Ra15,Rb6,X1,Z17), (Ra15,Rb6,X1,Z18), (Ra15,Rb6,X1,Z19), (Ra15,Rb6,X1,Z20), (Ra15,Rb6,X1,Z21), (Ra15,Rb6,X1,Z22), (Ra15,Rb6,X1,Z23), (Ra15,Rb6,X1,Z24), (Ra15,Rb6,X1,Z25), (Ra15,Rb6,X1,Z26), (Ra15,Rb6,X1,Z27), (Ra15,Rb6,X1,Z28), (Ra15,Rb6,X1,Z29), (Ra15,Rb6,X1,Z30), (Ra15,Rb6,X1,Z31), (Ra15,Rb6,X1,Z32), (Ra15,Rb6,X1,Z33), (Ra15,Rb6,X1,Z34), (Ra15,Rb6,X1,Z35), (Ra15,Rb6,X1,Z36), (Ra15,Rb6,X1,Z37), (Ra15,Rb6,X1,Z38), (Ra15,Rb6,X1,Z39), (Ra15,Rb6,X2,Z1), (Ra15,Rb6,X2,Z2), (Ra15,Rb6,X2,Z3), (Ra15,Rb6,X2,Z4), (Ra15,Rb6,X2,Z5), (Ra15,Rb6,X2,Z6), (Ra15,Rb6,X2,Z7), (Ra15,Rb6,X2,Z8), (Ra15,Rb6,X2,Z9), (Ra15,Rb6,X2,Z10), (Ra15,Rb6,X2,Z11), (Ra15,Rb6,X2,Z12), (Ra15,Rb6,X2,Z13), (Ra15,Rb6,X2,Z14), (Ra15,Rb6,X2,Z15), (Ra15,Rb6,X2,Z16), (Ra15,Rb6,X2,Z17), (Ra15,Rb6,X2,Z18), (Ra15,Rb6,X2,Z19), (Ra15,Rb6,X2,Z20), (Ra15,Rb6,X2,Z21), (Ra15,Rb6,X2,Z22), (Ra15,Rb6,X2,Z23), (Ra15,Rb6,X2,Z24), (Ra15,Rb6,X2,Z25), (Ra15,Rb6,X2,Z26), (Ra15,Rb6,X2,Z27), (Ra15,Rb6,X2,Z28), (Ra15,Rb6,X2,Z29), (Ra15,Rb6,X2,Z30), (Ra15,Rb6,X2,Z31), (Ra15,Rb6,X2,Z32), (Ra15,Rb6,X2,Z33), (Ra15,Rb6,X2,Z34), (Ra15,Rb6,X2,Z35), (Ra15,Rb6,X2,Z36), (Ra15,Rb6,X2,Z37), (Ra15,Rb6,X2,Z38), (Ra15,Rb6,X2,Z39), (Ra15,Rb7,X1,Z1), (Ra15,Rb7,X1,Z2), (Ra15,Rb7,X1,Z3), (Ra15,Rb7,X1,Z4), (Ra15,Rb7,X1,Z5), (Ra15,Rb7,X1,Z6), (Ra15,Rb7,X1,Z7), (Ra15,Rb7,X1,Z8), (Ra15,Rb7,X1,Z9), (Ra15,Rb7,X1,Z10), (Ra15,Rb7,X1,Z11), (Ra15,Rb7,X1,Z12), (Ra15,Rb7,X1,Z13), (Ra15,Rb7,X1,Z14), (Ra15,Rb7,X1,Z15), (Ra15,Rb7,X1,Z16), (Ra15,Rb7,X1,Z17), (Ra15,Rb7,X1,Z18), (Ra15,Rb7,X1, Z19), (Ra15,Rb7,X1,Z20), (Ra15,Rb7,X1,Z21), (Ra15,Rb7,X1,Z22), (Ra15,Rb7,X1,Z23), (Ra15,Rb7,X1,Z24), (Ra15,Rb7,X1,Z25), (Ra15,Rb7,X1,Z26), (Ra15,Rb7,X1,Z27), (Ra15,Rb7,X1,Z28), (Ra15,Rb7,X1,Z29), (Ra15,Rb7,X1,Z30), (Ra15,Rb7,X1,Z31), (Ra15,Rb7,X1,Z32), (Ra15,Rb7,X1,Z33), (Ra15,Rb7,X1,Z34), (Ra15,Rb7,X1,Z35), (Ra15,Rb7,X1,Z36), (Ra15,Rb7,X1,Z37), (Ra15,Rb7,X1,Z38), (Ra15,Rb7,X1,Z39), (Ra15,Rb7,X2,Z1), (Ra15,Rb7,X2,Z2), (Ra15,Rb7,X2,Z3), (Ra15,Rb7,X2,Z4), (Ra15,Rb7,X2,Z5), (Ra15,Rb7,X2,Z6), (Ra15,Rb7,X2,Z7), (Ra15,Rb7,X2,Z8), (Ra15,Rb7,X2,Z9), (Ra15,Rb7,X2,Z10), (Ra15,Rb7,X2,Z11), (Ra15,Rb7,X2,Z12), (Ra15,Rb7,X2,Z13), (Ra15,Rb7,X2,Z14), (Ra15,Rb7,X2,Z15), (Ra15,Rb7,X2,Z16), (Ra15,Rb7,X2,Z17), (Ra15,Rb7,X2,Z18), (Ra15,Rb7,X2,Z19), (Ra15,Rb7,X2,Z20), (Ra15,Rb7,X2,Z21), (Ra15,Rb7,X2,Z22), (Ra15,Rb7,X2,Z23), (Ra15,Rb7,X2,Z24), (Ra15,Rb7,X2,Z25), (Ra15,Rb7,X2,Z26), (Ra15,Rb7,X2,Z27), (Ra15,Rb7,X2,Z28), (Ra15,Rb7,X2,Z29), (Ra15,Rb7,X2,Z30), (Ra15,Rb7,X2,Z31), (Ra15,Rb7,X2,Z32), (Ra15,Rb7,X2,Z33), (Ra15,Rb7,X2,Z34), (Ra15,Rb7,X2,Z35), (Ra15,Rb7,X2,Z36), (Ra15,Rb7,X2,Z37), (Ra15,Rb7,X2,Z38), (Ra15,Rb7,X2,Z39), (Ra15,Rb8,X1,Z1), (Ra15,Rb8,X1,Z2), (Ra15,Rb8,X1,Z3), (Ra15,Rb8,X1,Z4), (Ra15,Rb8,X1,Z5), (Ra15,Rb8,X1,Z6), (Ra15,Rb8,X1,Z7), (Ra15,Rb8,X1,Z8), (Ra15,Rb8,X1,Z9), (Ra15,Rb8,X1,Z10), (Ra15,Rb8,X1,Z11), (Ra15,Rb8,X1,Z12), (Ra15,Rb8,X1,Z13), (Ra15,Rb8,X1,Z14), (Ra15,Rb8,X1,Z15), (Ra15,Rb8,X1,Z16), (Ra15,Rb8,X1,Z17), (Ra15,Rb8,X1,Z18), (Ra15,Rb8,X1,Z19), (Ra15,Rb8,X1,Z20), (Ra15,Rb8,X1,Z21), (Ra15,Rb8,X1,Z22), (Ra15,Rb8,X1,Z23), (Ra15,Rb8,X1,Z24), (Ra15,Rb8,X1,Z25), (Ra15,Rb8,X1,Z26), (Ra15,Rb8,X1,Z27), (Ra15,Rb8,X1,Z28), (Ra15,Rb8,X1,Z29), (Ra15,Rb8,X1,Z30), (Ra15,Rb8,X1,Z31), (Ra15,Rb8,X1,Z32), (Ra15,Rb8,X1,Z33), (Ra15,Rb8,X1,Z34), (Ra15,Rb8,X1,Z35), (Ra15,Rb8,X1,Z36), (Ra15,Rb8,X1,Z37), (Ra15,Rb8,X1,Z38), (Ra15,Rb8,X1,Z39), (Ra15,Rb8,X2,Z1), (Ra15,Rb8,X2,Z2), (Ra15,Rb8,X2,Z3), (Ra15,Rb8,X2,Z4), (Ra15,Rb8,X2,Z5), (Ra15,Rb8,X2,Z6), (Ra15,Rb8,X2,Z7), (Ra15,Rb8,X2,Z8), (Ra15,Rb8,X2,Z9), (Ra15,Rb8,X2,Z10), (Ra15,Rb8,X2,Z11), (Ra15,Rb8,X2,Z12), (Ra15,Rb8,X2,Z13), (Ra15,Rb8,X2,Z14), (Ra15,Rb8,X2,Z15), (Ra15,Rb8,X2,Z16), (Ra15,Rb8,X2,Z17), (Ra15,Rb8,X2,Z18), (Ra15,Rb8,X2,Z19), (Ra15,Rb8,X2,Z20), (Ra15,Rb8,X2,Z21), (Ra15,Rb8,X2,Z22), (Ra15,Rb8,X2,Z23), (Ra15,Rb8,X2,Z24), (Ra15,Rb8,X2,Z25), (Ra15,Rb8,X2,Z26), (Ra15,Rb8,X2,Z27), (Ra15, Rb8,X2,Z28), (Ra15,Rb8,X2,Z29), (Ra15,Rb8,X2,Z30), (Ra15,Rb8,X2,Z31), (Ra15,Rb8,X2,Z32), (Ra15,Rb8,X2,Z33), (Ra15,Rb8,X2,Z34), (Ra15,Rb8,X2,Z35), (Ra15,Rb8,X2,Z36), (Ra15,Rb8,X2,Z37), (Ra15,Rb8,X2,Z38), and (Ra15,Rb8,X2,Z39)

EXAMPLES

Following examples illustrate the present invention in more detail, but the present invention is not limited by these examples. The meaning of each abbreviation is following.

Me: methyl

Et: ethyl

Bu: butyl

Ac: acetyl

TMS: tetramethylsilane

TMS-Cl: trimethylsilyl chloride

DMSO: dimethyl sulfoxide

DMF: dimethylformamide

THF: tetrahydrofuran

rt: room temperature

Example 1
Preparation of 4-(2,2-dimethylpropionyl)-3-hydroxy-5-(2-methoxycarbonylmethyloxyphenyl-1-(4-thiophene-3-ylphenyl)-1,5-dihydropyrrole-2-one

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A mixture of ethyl trimethylacetopyruvate (0.40 g, 2 mmol), 4-thiophene-3-ylaniline (0.35 g, 2 mmol), 2-(methoxycarbonylmethyloxy)benzaldehyde (0.39, 2 mmol), acetic acid (0.057 mL, 1 mmol) and dioxane (4 mL) was heated at reflux overnight. After the reaction was completed, saturated sodium bicarbonate solution and brine were poured into the reaction mixture, and the resulting mixture was extracted with ethyl acetate. The extract was dried over anhydrous sodium sulphate, and then concentrated in vacuo. The resulting residue was purified on a silica gel column chromatography (methanol/chloroform), and the aimed compound was triturated with ethyl acetate and diisopropyl ether to give 4-(2,2-dimethylpropionyl)-3-hydroxy-5-(2-methoxycarbonylmethyloxyphenyl)-1-(4-thiophene-3-ylphenyl)-1,5-dihydropyrrole-2-one (0.42 g, yield: 41%) as pale brown solid.

1H-NMR (δ ppm TMS/DMSO-d6): 1.10 (9H, s), 3.78 (3H, s), 4.50-4.90 (2H, m), 6.00-6.45 (1H, m), 6.60-7.11 (11H, m).

Example 2
Preparation of 5-(2-hydroxycarbonylmethyloxyphenyl)-4-(2,2-dimethylpropionyl)-3-hydroxy-1-(4-thiophene-3-ylphenyl)-1,5-dihydropyrrole-2-one

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To a mixture of 4-(2,2-dimethylpropionyl)-3-hydroxy-5-(2-methoxycarbonylmethyloxyphenyl)-1-(4-thiophene-3-ylphenyl)-1,5-dihydropyrrole-2-one (0.172 g, 0.34 mmol), THF (1.72 mL), and methanol (1.72 mL) was added 1 mol/L aqueous lithium hydroxide solution (1.02 mL), and the resulting mixture was stirred at room temperature for 1 hour. After the reaction was completed, 2 mol/L hydrochloric acid (0.52 mL) and water (14 mL) were added to the reaction mixture, and the precipitated aimed compound was collected by filtration. The resulting aimed compound was dissolved in ethyl acetate, and the mixture was dried over anhydrous sodium sulphate and then concentrated in vacuo. The resulting residue was triturated with ethyl ether and diisopropyl ether to give 5-(2-hydroxycarbonylmethyloxyphenyl)-4-(2,2-dimethylpropionyl)-3-hydroxy-1-(4-thiophene-3-ylphenyl)-1,5-dihydropyrrole-2-one (0.137 g, yield: 82%) as pale yellow solid.

1H-NMR (δ ppm TMS/DMSO-d6): 1.10 (9H, s), 4.85 (2H, s), 6.46 (1H, brs), 6.76-7.75 (11H, m).

Example 3
Preparation of 3-t-butyl-5-(4-thiophene-3-ylphenyl)-4-(2-methoxycarbonylmethyloxyphenyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one

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A mixture of 4-(2,2-dimethylpropionyl)-3-hydroxy-5-(2-methoxycarbonylmethyloxyphenyl)-1-(4-thiophene-3-ylphenyl)-1,5-dihydropyrrole-2-one (0.207 g, 0.41 mmol), hydrazine hydrate (0.022 mL, 0.45 mmol) and acetic acid (3.1 mL) was stirred at 95° C. for 1 hour. After the reaction was completed, saturated sodium bicarbonate solution was poured into the reaction mixture, and the mixture was extracted with chloroform. The extract was washed with brine, dried over anhydrous sodium sulphate, and then concentrated in vacuo. The resulting residue was triturated with ethyl ether and diisopropyl ether to give 3-t-butyl-5-(4-thiophene-3-ylphenyl)-4-(2-methoxycarbonylmethyloxyphenyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one (0.191 g, yield: 93%) as pale brown solid.

1H-NMR (δ ppm TMS/DMSO-d6): 1.05 (9H, s), 3.78 (3H, s), 4.94 (2H, s), 6.70-7.77 (12H, m), 13.4 (1H, brs).

Example 4
Preparation of 3-t-butyl-5-(4-thiophene-3-ylphenyl)-4-(2-hydroxycarbonylmethyloxyphenyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one

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To a mixture of 3-t-butyl-5-(4-thiophene-3-ylphenyl)-4-(2-methoxycarbonylmethyloxyphenyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one (0.124 g, 0.25 mmol), THF (1.24 mL) and methanol (1.24 mL) was added 1 mol/L aqueous lithium hydroxide solution (0.74 mL), and the resulting mixture was stirred at room temperature for 1.5 hours. After the reaction was completed, 2 mol/L hydrochloric acid (0.38 mL) and water (10 mL) were poured into the reaction mixture, and the precipitated aimed compound was collected by filtration. The resulting aimed compound was dissolved in ethyl acetate, and the solution was dried over anhydrous sodium sulphate and then concentrated in vacuo. The resulting residue was triturated with ethyl ether and diisopropyl ether to give 5-(2-hydroxycarbonylmethyloxyphenyl)-4-(2,2-dimethylpropionyl)-3-hydroxy-1-(4-thiophene-3-ylphenyl)-1,5-dihydropyrrole-2-one (0.104 g, yield: 87%) as pale brown solid.

1H-NMR (δ ppm TMS/DMSO-d6): 1.05 (9H, s), 4.78 (2H, s), 6.70-7.80 (12H, m), 13.33 (1H, brs).

Example 5
Preparation of 1-(6-furan-3-yl-3-pyridyl)-4-(2,2-dimethylpropionyl)-3-hydroxy-5-(2-methoxy-3-pyridyl)-1,5-dihydropyrrole-2-one

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A mixture of 1-(6-bromo-3-pyridyl)-4-(2,2-dimethylpropionyl)-3-hydroxy-5-(2-methoxy-3-pyridyl)-1,5-dihydropyrrole-2-one (0.10 g, 0.22 mmol), furan-3-yl boronic acid (0.038 g, 0.34 mmol), tripotassium phosphate (0.14 mg, 0.67 mmol), 1,2-Dimethoxyethane (3 mL) and water (0.6 mL) was placed in a flask under nitrogen. To the mixture was added 1,1′-Bis(diphenylphosphino)ferrocene-palladium(II)dichloride dichloromethane complex (0.018 g, 0.022 mmol), and the resulting mixture was heated at reflux for 4 hours. After the reaction was completed, saturated ammonium chloride aqueous solution was poured into the mixture and the resulting mixture was extracted with ethyl acetate. The extract was washed with brine, dried over anhydrous sodium sulphate, and concentrated in vacuo. The resulting residue was purified on a silica gel column chromatography (ethyl acetate/n-hexane) and the aimed compound was triturated with ethyl acetate and n-hexane to give 1-(6-furan-3-yl-3-pyridyl)-4-(2,2-dimethylpropionyl)-3-hydroxy-1-5-(2-methoxy-3-pyridyl)-1,5-dihydropyrrole-2-one (0.045 g, yield: 46%) as colorless solid.

1H-NMR (δ ppm TMS/DMSO-d6): 1.11 (9H, s), 3.79 (3H, brs), 6.24 (1H, brs), 6.86 (1H, m), 6.96 (1H, m), 7.64-7.95 (4H, m), 8.23 (1H, s), 8.71 (1H, s), 12.31 (1H, brs).

Example 6
Preparation of 3-t-butyl-5-(6-thiophene-2-yl-3-pyridyl)-4-(2-methoxy-3-pyridyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one

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A mixture of 5-(6-bromo-3-pyridyl)-3-t-butyl-4-(2-methoxy-3-pyridyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one (0.10 g, 0.23 mmol), thiophene-2-yl boronic acid (0.043 g, 0.34 mmol), tripotassium phosphate (0.14 mg, 0.67 mmol), 1,2-Dimethoxyethane (3 mL) and water (0.6 mL) was placed in a flask under nitrogen. To the mixture was added 1,1′-Bis(diphenylphosphino)ferrocene-palladium(II) dichloride dichloromethane complex (0.018 g, 0.022 mmol) and the resulting mixture was heated at reflux for 3 hours. After the reaction was completed, water was added to the mixture, and the resulting mixture was extracted with ethyl acetate. The extract was dried over anhydrous sodium sulphate and concentrated in vacuo. The resulting residue was purified on a silica gel column chromatography (ethyl acetate/n-hexane). The aimed compound was triturated with ethyl acetate and n-hexane to give 1-(6-furan-3-yl-3-pyridyl)-4-(2,2-dimethylpropionyl)-3-hydroxy-1-5-(2-methoxy-3-pyridyl)-1,5-dihydropyrrole-2-one (0.089 g, yield: 88%) as colorless solid.

1H-NMR (δ ppm TMS/DMSO-d6): 1.07 (9H, s), 3.97 (3.55) (3H, s), 6.56-7.28 (4H, m), 7.58 (1H, d, J=5.0), 7.69 (1H, d, J=3.7), 7.87-8.10 (3H, m), 8.64 (1H, s), 13.36 (1H, m).

Example 7
Preparation of 3-(1-hydroxymethyl-1-methylethyl)-4-(2-methoxyphenyl)-5-(4-thiophene-3-ylphenyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one

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A mixture of methyl 5,5-dimethyl-2,4-dioxo-6-(tetrahydro-2H-pyrane-2-yloxy)hexanoate (4.29 g, 15 mmol), 4-bromoaniline (2.58 g, 15 mmol), 2-methoxybenzaldehyde (1.812 mL, 15 mmol), acetic acid (0.343 mL, 6 mmol) and dioxane (15 ml) was heated at reflux overnight. After the reaction was completed, the mixture was concentrated in vacuo and the resulting residue was purified on a silica gel column chromatography (ethyl acetate/n-hexane). The resulting aimed compound was triturated with ethyl acetate and n-hexane to give 1-(4-bromophenyl)-4-(2,2-dimethyl-3-tetrahydro-2H-pyrane-2-yloxypropionyl)-3-hydroxy-5-(2-methoxyphenyl)-1,5-dihydropyrrole-2-one (2.69 g, yield: 33%) as colorless solid.

1H-NMR (δ ppm TMS/DMSO-d6): 1.08 (3H, s), 1.13 (3H, s), 1.20-1.40 (6H, m), 3.50-3.90 (7H, m), 4.37 (1H, m), 6.31 (1H, brs), 6.70-7.44 (8H, m), 12.23 (1H, brs).

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A mixture of 1-(4-bromophenyl)-4-(2,2-dimethyl-3-tetrahydro-2H-pyrane-2-yloxypropionyl)-3-hydroxy-5-(2-methoxyphenyl)-1,5-dihydropyrrole-2-one (1.51 g, 2.77 mmol), hydrazine hydrate (0.204 mL, 4.16 mmol) and acetic acid (3 mL) was stirred at 95° C. for 2 hours. After the reaction was completed, saturated sodium bicarbonate solution (150 mL) was poured into the reaction mixture, and the resulting mixture was extracted with ethyl acetate. The extract was washed with saturated sodium bicarbonate solution, dried over anhydrous sodium sulphate, and concentrated in vacuo. The resulting residue was triturated with ethyl acetate to give 5-(4-bromophenyl)-3-(1-hydroxymethyl-1-methylethyl)-4-(2-methoxyphenyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one (1.02 g, yield: 81%) as colorless solid.

1H-NMR (δ ppm TMS/DMSO-d6): 0.88 (3H, s), 1.00 (3H, s), 3.11 (2H, m), 3.87 (3H, s), 4.73 (1H, brs), 6.30-7.50 (9H, m), 13.21 (1H, m).

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A mixture of 5-(4-bromophenyl)-3-(1-hydroxymethyl-1-methylethyl)-4-(2-methoxyphenyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one (0.15 g, 0.33 mmol), thiophene-3-yl boronic acid (0.063. g, 0.49 mmol), tripotassium phosphate (0.21 mg, 0.99 mmol), 1,2-Dimethoxyethane (3 mL) and water (0.6 mL) was placed in a flask under nitrogen. To the mixture was added 1,1′-Bis(diphenylphosphino)ferrocene-palladium(II) dichloride dichloromethane complex (0.027 mg, 0.033 mmol) and the resulting mixture was heated at reflux for 5 hours. After the reaction was completed, the reaction mixture was purified on a silica gel column chromatography (ethyl acetate/n-hexane). The resulting aimed compound was triturated with ethyl acetate and n-hexane to give 3-(1-hydroxymethyl-1-methylethyl)-4-(2-methoxyphenyl)-5-(4-thiophene-3-ylphenyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one (0.038 g, yield: 25%) as colorless solid.

1H-NMR (5 ppm TMS I DMSO-d6): 0.91 (3H, s), 1.04 (3H, s), 3.25 (2H, m), 3.91 (3H, s), 4.74 (1H, s), 6.33-7.78 (9H, m), 13.21 (1H, m)

Example 8
Preparation of 3-(1-hydroxymethyl-1-methylethyl)-4-(2-methoxy-3-pyridyl)-5-(4-thiophene-3-ylphenyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one

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A mixture of methyl 5,5-dimethyl-2,4-dioxo-6-(tetrahydro-2H-pyrane-2-yloxy)hexanoate (0.29 mg, 1.0 mmol), 4-(3-thienyl)aniline (0.18 g, 1.0 mmol), 2-methoxynicotinaldehyde (0.14 g, 1.0 mmol), acetic acid (0.043 mL, 0.75 mmol) and dioxane (2 ml) was heated at reflux overnight. After the reaction was completed, the reaction mixture was concentrated in vacuo. The resulting residue was purified on a silica gel column chromatography (methanol/chloroform) to give 4-(2,2-dimethyl-3-tetrahydro-2H-pyrane-2-yloxypropionyl)-3-hydroxy-5-(2-methoxy-3-pyridyl)-1-(4-thiophene-3-ylphenyl)-1,5-dihydropyrrole-2-one (0.30 g, yield: 55%) as pale yellow solid.

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To a mixture of 4-(2,2-dimethyl-3-tetrahydro-2H-pyrane-2-yloxypropionyl)-3-hydroxy-5-(2-methoxy-3-pyridyl)-1-(4-thiophene-3-ylphenyl)-1,5-dihydropyrrole-2-one (0.30 g, 0.55 mmol), methanol (3 mL) and chloroform (3 mL) was added p-toluenesulfonic acid hydrate (0.158 g, 0.8 mmol), and the resulting mixture was stirred at room temperature for 3 hours. After the reaction was completed, saturated sodium bicarbonate solution and brine were poured into the mixture. The resulting mixture was extracted with chloroform. The extract was dried over anhydrous sodium sulphate and concentrated in vacuo. To the obtained crude 4-(2,2-dimethyl-3-hydroxypropionyl)-3-hydroxy-5-(2-methoxy-3-pyridyl)-1-(4-thiophene-3-ylphenyl)-1,5-dihydropyrrole-2-one (0.233 g), acetic acid (2 mL) and hydrazine hydrate (0.074 mL, 1.5 mmol) were added, and the resulting mixture was stirred at 50° C. for 1 hour. After the reaction was completed, saturated sodium bicarbonate solution was poured into the mixture, and the resulting mixture was extracted with chloroform. The extract was dried over anhydrous sodium sulphate and concentrated in vacuo. The resulting residue was triturated with ethyl acetate to give 3-(1-hydroxymethyl-1-methylethyl)-4-(2-methoxy-3-pyridyl)-5-(4-thiophene-3-ylphenyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one (0.061 g, yield: 26%) as colorless solid.

1H-NMR (δ ppm TMS/DMSO-d6): 0.95 (3H, s), 1.06 (3H, s), 3.23 (2H, m), 4.06 (213, s), 4.78 (1H, brs), 6.43-8.10 (10H, m), 13.40 (1H, m).

Example 9
Preparation of 3-(1,1-dihydroxymethylethyl)-4-(2-methoxyphenyl)-5-(4-thiophene-3-ylphenyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one

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To a mixture of 3-hydroxy-2-hydroxymethyl-2-methylpropionic acid (6.71 g, 50 mmol), dimethoxypropane (7.99 mL, 65 mmol) and acetone (50 mL), p-toluenesulfonic acid hydrate (0.048 g, 0.25 mmol) was added and the resulting mixture was stirred at room temperature for 2.5 hours. After the reaction was completed, sodium bicarbonate (0.1 g) was added to the reaction mixture, and the resulting mixture was stirred at room temperature for 5 minutes and concentrated in vacuo. To the resulting residue was added water and the resulting mixture was extracted with ethyl ether. The extract was dried over anhydrous sodium sulphate and concentrated in vacuo to give 2,2,5-trimethyl-1,3-dioxane5-carboxylic acid (7.87 g, yield: 90%) as colorless oil.

1H-NMR (δ ppm TMS/CDCl3): 1.20 (3H, s), 1.43 (3H, s), 1.46 (3H, s), 3.70 (2H, d, J=11.7), 4.16 (2H, d, J=11.7).

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To a mixture of 2,2,5-trimethyl-1,3-dioxane5-carboxylic acid (1.0 g, 5.74 mmol) and DMF (10 mL) were added N,O-dimethylhydroxylamine hydrochloride (0.84 g, 8.6 mmol), 1-hydroxybenzotriazole hydrate (1.32 g, 8.6 mmol), 1-ethyl-3-(3-dimethylaminopropyl)carbodiimide hydrochloric acid (1.651 g, 8.61 mmol) and triethylamine (2.39 mL, 17.2 mmol) under nitrogen atmosphere, and the resulting mixture was stirred at room temperature for 3 hours. After the reaction was completed, water was added to the reaction mixture and the resulting mixture was extracted with ethyl acetate. The extract was washed with brine, dried over anhydrous sodium sulphate, and concentrated in vacuo to give N-methoxy-N,2,2,5-tetramethyl-1,3-dioxane5-carboxylic acid amid (1.08 g, yield: 86%) as colorless oil.

1H-NMR (δ ppm TMS/CDCl3): 1.38 (3H, s), 1.41 (3H, s), 1.42 (3H, s), 3.18 (3H, s), 3.69 (3H, s), 3.76 (2H, d, J=11.7), 4.19 (2H, d, J=11.7).

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To a mixture of N-methoxy-N,2,2,5-tetramethyl-1,3-dioxane5-carboxylic acid amid (1.07 g, 4.92 mmol) and THF (10 mL) was gradually added 3 mol/L methylmagnesium bromide in THF (2.46 mL, 7.4 mmol) at 0° C. under nitrogen atmosphere, and the resulting mixture was stirred at 0° C. for 4 hours. After the reaction was completed, saturated ammonium chloride aqueous solution was added to the reaction mixture and the resulting mixture was extracted with ethyl acetate. The extract was washed with brine, dried over anhydrous sodium sulphate, and concentrated in vacuo to give 1-(2,2,5-trimethyl-1,3-dioxane5-yl)ethanone (0.76 g, yield: 90%) as colorless oil.

1H-NMR (δ ppm TMS/CDCl3): 1.03 (3H, s), 1.37 (3H, d, J=0.5), 1.45 (3H, d, J=0.5), 2.28 (3H, s), 3.68 (2H, d, J=12.2), 4.16 (2H, d, J=12.2).

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To a mixture of 1-(2,2,5-trimethyl-1,3-dioxane5-yl)ethanone (0.76 g, 4.4 mmol) and THF (7.6 mL) was added sodium hydride (0.16 g, 6.6 mmol) under nitrogen atmosphere, and the resulting mixture was stirred at room temperature for 0.5 hour. To the resulting reaction mixture was added dimethyl oxalate (0.78 g, 6.6 mmol) and the mixture was heated at reflux for 2 hours. After the reaction was completed, saturated ammonium chloride aqueous solution was added to mixture and the resulting mixture was extracted with ethyl acetate. The extract was washed with brine, dried over anhydrous sodium sulphate, and concentrated in vacuo. The resulting residue was purified on a silica gel column chromatography (ethyl acetate/n-hexane) to give methyl 2,4-dioxo-4-(2,2,5-trimethyl-1,3-dioxane5-yl)butanoate (1.0 g, yield: 88%) as colorless oil.

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A mixture of methyl 2,4-dioxo-4-(2,2,5-trimethyl-1,3-dioxane5-yl)butanoate (0.26 mg, 1.0 mmol), 4-(3-thienyl)aniline (0.18 g, 1.0 mmol), 2-methooxybenzaldehyde (0.12 mL, 1.0 mmol), acetic acid (0.023 mL, 0.40 mmol) and dioxane (2 ml) was heated at reflux overnight. After the reaction was completed, the mixture was concentrated in vacuo. To the residue was added diisopropyl ether, and the resulting mixture was stirred under ice-cooling. The precipitated aimed compound was collected by filtration to give 3-hydroxy-4-(2,2,5-trimethyl-1,3-dioxane5-yl)carbonyl-5-(2-methoxyphenyl)-1-(4-thiophene-3-ylphenyl)-1,5-dihydropyrrole-2-one (0.29 g, yield: 56%) as pale yellow solid.

1H-NMR (δ ppm TMS/CDCl3): 0.99 (3H, s), 1.12 (3H, s), 1.40 (3H, s), 3.63-3.76 (2H, m), 3.89 (3H, brs), 4.20-4.37 (2H, m), 6.50-7.58 (12H, m), 9.00 (1H, brs).

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A mixture of 3-hydroxy-4-(2,2,5-trimethyl-1,3-dioxane5-yl)carbonyl-5-(2-methoxyphenyl)-1-(4-thiophene-3-ylphenyl)-1,5-dihydropyrrole-2-one (0.15 g, 0.3 mmol), hydrazine hydrate (0.07 mL, 1.4 mmol) and acetic acid (1 mL) was heated at reflux overnight. After the reaction mixture was concentrated in vacuo, to the resulting residue was added 2 mol/L hydrochloric acid/methanol solution (2.89 mL, 5.8 mmol) and the resulting mixture was heated at reflux for 6 hours. After the reaction mixture was concentrated in vacuo, saturated sodium bicarbonate solution was added to the residue and the mixture was extracted with chloroform. The extract was dried over anhydrous magnesium sulfate and concentrated in vacuo. The resulting residue was purified on a silica gel column chromatography (methanol/chloroform). The resulting compound was triturated with ethyl acetate and n-hexane to give 3-(1,1-dihydroxymethylethyl) 4-(2-methoxyphenyl)-5-(4-thiophene-3-ylphenyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one (0.105 g, yield: 77%) as colorless solid.

1H-NMR (δ ppm TMS/DMSO-d6): 0.95 (3H, s), 3.91 (2H, m), 4.57 (2H, m), 6.29-7.78 (12H, m), 12.97 (1H, m).

Example 10
Preparation of 3-(1-hydroxy carbonyl-1-methylethyl)-5-(4-isoxazolyl-3-ylphenyl)-4-(2-methoxyphenyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one

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To a solution of periodic acid (0.32 mg, 1.4 mmol) in acetonitrile (15 mL), a solution of 3-(1-hydroxymethyl-1-methylethyl)-5-(4-isoxazolyl-3-ylphenyl)-4-(2-methoxyphenyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one (0.206 g, 0.463 mmol) in dichloromethane (15 mL) and pyridiniumchlorochromate (0.01 g, 0.046 mmol) were added, and the resulting mixture was stirred at room temperature for 4 hours. After the reaction was completed, water was added to the reaction mixture, and the resulting mixture was extracted with ethyl acetate. The extract was washed with brine, and dried over anhydrous sodium sulphate, and then concentrated in vacuo. To the resulting residue was added dichloromethane, and the precipitated compound was collected by filtration to give 3-(1-hydroxy carbonyl-1-methylethyl)-5-(4-isoxazolyl-3-ylphenyl)-4-(2-methoxyphenyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one (0.11 g, yield: 49%) as pale yellow solid.

1H-NMR (8 ppm TMS/DMSO-d6): 1.19 (3H, s), 1.30 (3H, s), 3.91 (3H, brs), 6.40-7.19 (6H, m), 7.66-7.80 (4H, m), 8.94 (1H, d, J=1.7), 12.50 (1H, brs), 13.55 (1H, brs).

Example 11
Preparation of 5-(4-isoxazolyl-3-ylphenyl)-4-(2-methoxyphenyl)-3-[1-(N-methylcarbamoyl)-1-methylethyl]-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one

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To a mixture of 3-(1-hydroxy carbonyl-1-methylethyl)-5-(4-isoxazolyl-3-ylphenyl)-4-(2-methoxyphenyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one (0.05 g, 0.11 mmol) and DMF (2 mL) were added methylamine hydrochloride (0.013 g, 0.19 mmol), 1-hydroxybenzotriazole (0.039 g, 0.29 mmol), 4-dimethylaminopyridine (0.005 g, 0.04 mmol), 1-ethyl-3-(3-dimethylaminopropyl)carbodiimide hydrochloric acid (0.058 g, 0.3 mmol) and triethylamine (0.040 mL, 0.29 mmol), and the resulting mixture was stirred at room temperature for 2 hours. After the reaction was completed, water (2 mL) was added to the reaction mixture, and the resulting mixture was stirred under ice-cooling for a while. The precipitated compound was filtered off, and the residue was purified on a silica gel column chromatography (ethyl acetate/n-hexane) to give 5-(4-isoxazolyl-3-ylphenyl)-4-(2-methoxyphenyl)-3-[1-(N-methylcarbamoyl)-1-methylethyl]-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one (0.036 g, yield: 40%) as pale brown solid.

1H-NMR (δ ppm TMS/DMSO-d6) 1.12 (3H, s), 1.29 (3H, s), 2.43 (3H, brs), 3.91 (3H, brs), 6.63-7.20 (7H, m), 7.67-7.82 (4H, m), 8.95 (1H, d, J=1.7), 13.43 (1H, brs).

Example 12
Preparation of (−)-4-(2-methylpropionyl)-3-hydroxy-1-(4-bromophenyl)-5-(2-methoxyphenyl)-1,5-dihydropyrrole-2-one

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To a mixture of 4-(2-methylpropionyl)-3-hydroxy-1-(4-bromophenyl)-5-(2-methoxyphenyl)-1,5-dihydropyrrole-2-one (2.15 g, 5 mmol), (R)-methyl 2-hydroxy-2-phenylacetate (1.00 g, 6.0 mmol), triphenylphosphine (1.44 g, 5.5 mmol) and dioxane (15 mL) was added dimethoxyethyl azodicarboxylate (1.29 g, 5.5 mmol) at room temperature over 1 minute, and the resulting mixture was stirred at room temperature for 6 hours. To the reaction mixture was added water (200 mL) and the resulting mixture was extracted with ethyl acetate (200 mL). The extract was washed with brine (200 mL), dried over anhydrous magnesium sulfate, and concentrated in vacuo. The resulting residue was purified on a silica gel column chromatography (ethyl acetate/n-hexane). The resulting mixture of diastereomers was recrystallized (ethyl acetate/n-hexane) to give the diastereomer (0.80 g, yield: 28%) as pale yellow crystalline.

A mixture of the resulting diastereomer (0.59 g, 1 mmol), lithium chloride (0.127 g, 3 mmol) and 1,3-dimethyl-2-imidazolidinone (3 mL) was stirred at 80° C. for 6 hours. To the reaction mixture were added water (200 mL) and 1 mol/L hydrochloric acid (3 mL), and the resulting mixture was extracted with toluene (200 mL). The extract was washed with brine (200 mL), dried over anhydrous magnesium sulfate, and concentrated in vacuo. The resulting residue was purified on a silica gel column chromatography (ethyl acetate/n-hexane). The resulting compound was recrystallized (ethyl acetate/n-hexane) to give (−)-4-(2-methylpropionyl)-3-hydroxy-1-(4-bromophenyl)-5-(2-methoxyphenyl)-1,5-dihydropyrrole-2-one (0.40 g, yield: 93%) as pale yellow crystalline.

[α]_D: −142.2±3.6° (in CHCl3),

1H-NMR (δ ppm TMS/DMSO-d6) 0.88 (3H, d, J=6.9), 0.91 (3H, d, J=6.9), 3.33 (1H, sept, J=6.9), 3.81 (3H, brs), 6.23 (1H, brs), 6.75-7.15 (4H, m), 7.45-7.53 (4H, m), 12.00 (1H, brs).

Example 13
Preparation of (−)-4-(2-methylpropionyl)-3-hydroxy-1-(4-thiophene-3-ylphenyl)-5-(2-methoxyphenyl)-1,5-dihydropyrrole-2-one

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After a mixture of (−)-4-(2-methylpropionyl)-3-hydroxy-1-(4-bromophenyl)-5-(2-methoxyphenyl)-1,5-dihydropyrrole-2-one (0.10 g, 0.23 mmol), 3-thiophene-boronic acid (0.045 g, 0.35 mmol), tripotassium phosphate (0.148 g, 0.7 mmol), 1,2-dimethoxyethane (3 mL) and water (3 mL) was placed in a flask under nitrogen, 1,1′-Bis(diphenylphosphino)ferrocene-palladium(II)dichloride dichloromethane complex (0.019 g, 0.023 mmol) was added to the mixture, and the resulting mixture was stirred at reflux for 3 hours. To the reaction mixture was added water (50 mL), and the resulting mixture was extracted with dichloromethane (50 mL). The extract was washed with brine (50 mL), dried over anhydrous magnesium sulfate, and concentrated in vacuo. The resulting residue was purified on a silica gel column chromatography (methanol/chloroform). The resulting compound was triturated with ethyl acetate/n-hexane to give (−)-4-(2-methylpropionyl)-3-hydroxy-1-(4-thiophene-3-ylphenyl)-5-(2-methoxyphenyl)-1,5-dihydropyrrole-2-one (0.029 g, yield: 29%) as pale brown powder.

[α]_D: −57.4+1.9° (in CHCl3),

1H-NMR (δ ppm TMS/DMSO-d6) 0.89 (3H, d, J=6.9), 0.92 (3H, d, J=6.9), 3.34 (1H, sept, J=6.9), 3.87 (3H, brs), 6.32 (1H, brs), 6.75-7.15 (5H, m), 7.51 (1H, d, J=1.1), 7.58-7.63 (4H, m), 7.81 (1H, m), 12.00 (1H, brs).

Example 14
Preparation of 3-i-prppyl-5-(4-thiophene-3-ylphenyl)-4-(2-methoxyphenyl)-1,4,5,6-tetrahydro-1H-pyrrolo[3,4-c]pyrazole

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To a mixture of 3-i-propyl-5-(4-thiophene-3-ylphenyl)-4-(2-methoxyphenyl)-4,5-dihydro-1H-pyrrolo[3,4-c]pyrazole-6-one (0.72 g, 1.65 mmol) and dioxane (40 mL), lithium aluminum hydride (0.19 g, 5 mmol) was added and the resulting mixture was heated at reflux for 2 hours. The reaction mixture was added to a mixture of ice-water (100 mL) and 2 mol/L hydrochloric acid (10 mL), and the resulting mixture was extracted with chloroform (100 mL). The extract was washed with brine (100 mL), and dried over anhydrous sodium sulphate, and concentrated in vacuo. The resulting residue was purified on a silica gel column chromatography (methanol/chloroform). The resulting compound was triturated with ether to give 3-i-propyl-5-(4-thiophene-3-ylphenyl)-4-(2-methoxyphenyl)-1,4,5,6-tetrahydro-1H-pyrrolo[3,4-c]pyrazole (0.029 g, yield: 29%) as pale brown powder.

1H-NMR (δ ppm TMS/DMSO-d6) 0.86 (3H, d, J=7.0), 0.97 (3H, d, J=7.0), 2.78 (1H, sept, J=7.0), 3.94 (3H, s), 4.42 (1H, d, J=12.6), 4.77 (1H, d, J=12.6), 6.11 (1H, d, J=2.0), 6.55-7.53 (11H, m), 12.32 (1H, s).

Example 15
Preparation of (−)-4-(2-methylpropionyl)-3-hydroxy-1-(4-thiophene-3-ylphenyl)-5-(2-methoxyethoxyphenyl)-1,5-dihydropyrrole-2-one

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To a mixture of 4-(2-methylpropionyl)-3-hydroxy-1-(4-bromophenyl)-5-(2-methoxymethylphenyl)-1,5-dihydropyrrole-2-one (11.0 g, 23.7 mmol), (R)-methyl 2-hydroxy-2-phenylacetate (4.73 g, 28.5 mmol), triphenylphosphine (7.47 g, 28.5 mmol) and THF (150 mL) was added dimethoxyethyl azodicarboxylate (6.67 g, 28.5 mmol) at room temperature over 2 minutes, and the resulting mixture was stirred at room temperature overnight. To the reaction mixture was added water (200 mL), and the resulting mixture was extracted with toluene (200 mL). The extract was washed with brine (200 mL), dried over anhydrous magnesium sulfate, and concentrated in vacuo. The resulting residue was purified on a silica gel column chromatography (ethyl acetate/n-hexane). The resulting mixture of diastereomers was recrystallized by ethyl acetate/n-hexane to give diastereomer A (4.98 g, yield: 34%) as pale yellow crystalline.

1H-NMR (δ ppm TMS/CDCl3) 0.85 (3H, d, J=7.0), 1.15 (3H, d, J=7.0), 3.49 sept, J=7.0), 3.57 (3H, brs), 3.73 (3H, s), 5.25 (2H, brs), 6.40-6.80 (2H, m), 7.05-7.63 (16H, m).

To a solution of Diastereomer A (4.0 g, 6.5 mmol) in ethyl acetate (33 mL) was added 2 mol/l hydrochloric acid/methanol solution (32.7 mL), and the resulting mixture was stirred at 60° C. for 1 hour. To the reaction mixture was added water (200 mL), the resulting mixture was extracted with ethyl acetate (200 mL). The extract was washed with brine (200 mL), dried over anhydrous magnesium sulfate, and concentrated in vacuo. The resulting residue was purified on a silica gel column chromatography (ethyl acetate/n-hexane). The resulting mixture of diastereomers was triturated with ethyl acetate/n-hexane to give diastereomer B (2.93 g, yield: 79%) as yellow powder.

1H-NMR (δ ppm TMS/CDCl3) 0.90 (3H, d, J=6.9), 1.24 (3H, d, J=6.9), 3.52 (1H, sept, J=6.9), 3.75 (3H, s), 6.22 (1H, s), 6.68-6.75 (2H, m), 6.97-7.56 (15H, m), 7.95 (1H, s).

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To a mixture of Diastereomer B (2.65 g, 4.7 mmol), 2-methoxyethanol (0.71 g, 9.3 mmol), triphenylphosphine (1.84 g, 7.0 mmol) and THF (50 mL) was added dimethoxyethyl azodicarboxylate (1.64 g, 7.0 mmol) at room temperature over 2 minutes, and the resulting mixture was stirred at room temperature overnight. To the reaction mixture was added water (200 mL), and the resulting mixture was extracted with toluene (200 mL). The extract was washed with brine (200 mL), dried over anhydrous magnesium sulfate, and concentrated in vacuo. The resulting residue was purified on a silica gel column chromatography (ethyl acetate/n-hexane) to give diastereomer C (2.44 g, yield: 84%) as yellow amorphous.

A mixture of the obtained diastereomer C (2.25 g, 3.6 mmol), lithium chloride (0.46 g, 10.8 mmol) and 1,3-dimethyl-2-imidazolidinone (45 mL) was stirred at 100° C. for 16 hours. To the reaction mixture were added water (200 mL) and 2 mol/L hydrochloric acid (15 mL), and the resulting mixture was extracted with toluene (200 mL). The extract was washed with brine (200 mL), dried over anhydrous magnesium sulfate, and concentrated in vacuo. The resulting residue was purified on a silica gel column chromatography (methanol/chloroform). The resulting compound was triturated with ethyl acetate/n-hexane to give (−)-4-(2-methylpropionyl)-3-hydroxy-1-(4-thiophene-3-ylphenyl)-5-(2-methoxyethoxyphenyl)-1,5-dihydropyrrole-2-one (1.01 g, yield: 59%) as pale yellow powder.

[α]_D: −39.3±1.6° (in CHCl3),

1H-NMR (δ ppm TMS/DMSO-d6) 0.89 (3H, d, J=7.0), 0.93 (3H, d, J=7.0), 3.44 (3H, s), 3.57 (2H, brs), 3.83 (3H, s), 4.15 (1H, m), 4.29 (1H, m), 6.01 (1H, s), 6.38 (1H, s), 6.63-7.13 (4H, m), 7.40-7.76 (7H, m), 7.78 (1H, m), 12.5 (1H, brs)

Example 16
Preparation of 4-(i-propylsulfonyl)-3-hydroxy-1-(4-thiophene-3-ylphenyl)-5-(2-methoxyphenyl)-1,5-dihydropyrrole-2-one

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To a mixture of i-propylmethylsulfone (5.17 g, 42.3 mmol) and THF (20 mL) was added 28% sodium methoxide methanol solution (8.58 g, 44.5 mmol) at room temperature, and then methyl oxalate (5.0 g, 42.3 mmol) was gradually added to the mixture at room temperature. The resulting mixture was stirred at room temperature overnight. To the reaction mixture was added ice-water (200 mL), and the pH of the resulting mixture was adjusted pH3 or less than pH3 with 2 mol/L hydrochloric acid. The mixture was extracted with ethyl acetate (200 mL). The extract was washed with brine (200 mL), dried over anhydrous sodium sulphate, and concentrated in vacuo. The resulting residue was purified on a silica gel column chromatography (ethyl acetate/n-hexane) to give methyl 3-(i-propylsulfonyl)-2-oxopropanoate (2.7 g, yield: 28%) as colorless oil.

1H-NMR (δ ppm TMS/DMSO-d6) 1.26 (6H, d, J=6.7), 3.46 (1H, sept, J=6.7), 3.81 (3H, s), 4.74 (2H, s).

A mixture of methyl 3-(i-propylsulfonyl)-2-oxopropanoate (0.23 g, 1 mmol), 4-thiophene-3-ylaniline (0.18 g, 1 mmol), 2-methoxybenzaldehyde (0.14, 1 mmol), acetic acid (0.023 mL, 0.4 mmol) and toluene (3 mL) was heated at reflux overnight. After the reaction was completed, the reaction mixture was allowed to cool to room temperature. To the mixture was added ether and precipitated compound was collected by filtration. The resulting aimed compound was washed with ether/n-hexane solution to give 4-(i-propylsulfonyl)-3-hydroxy-1-(4-thiophene-3-ylphenyl)-5-(2-methoxyphenyl)-1,5-dihydropyrrole-2-one (0.37 g, yield: 79%) as pale brown solid.

1H-NMR (δ ppm TMS/DMSO-d6): 0.97-1.15 (6H, m), 3.62 (3.87) (3H, s), 6.13 (6.50) (1H, s), 6.82-7.27 (3H, m), 7.48-7.81 (8H, m), 12.20 (1H, brs).

The following compounds were synthesized in a manner similar to those described in the above synthetic scheme, general, general procedures for the synthesis of the compound of the invention, and Examples. The chemical structure of the compounds and the physical properties of them are described below.

(Method of Identification for the Compound)

LC/MS data of compound of the present invention were measured under any one of the following 2 conditions (Method 1 to 3), and a retention time and [M+H]⁺ are shown.

(Method 1)

Column: Xbridge C18(5 μm, i.d. 4.6×50 mm) (Waters)

Flow rate: 3 mL/min

UV detection wavelength: 254 nm

Mobile phase: [A] is 0.1% formic acid-containing aqueous solution, and [B] is 0.1% formic acid-containing acetonitrile solution

Gradient: Linear gradient of 10% to 100% solvent[B] for 3 minutes was performed, and 100% solvent [B] was maintained for 1 minute.

(Method 2)

Column: Shim-pack XR-ODS (2.2 μm, i.d. 50×3.0 mm) (Shimadzu)

Flow rate: 1.6 mL/min

UV detection wavelength: 254 nm

Mobile phase: [A] is 0.1% formic acid-containing aqueous solution, and [B] is 0.1% formic acid-containing acetonitrile solution

Gradient: Linear gradient of 10% to 100% solvent[B] for 3 minutes was performed, and 100% solvent [B] was maintained for 1 minute.

(Method 3)

Column: Gemini-NX (5 μm, i.d. 4.6×50 mm) (Phenomenex)

Flow rate: 3 mL/min

UV detection wavelength: 254 nm

Mobile phase: [A] is 0.1% formic acid-containing aqueous solution, and [B] is 0.1% formic acid-containing acetonitrile solution

Gradient: Linear gradient of 10% to 100% solvent[B] for 3.5 minutes was performed, and 100% solvent [B] was maintained for 0.5 minute.

TABLE 10

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

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I-001
438
2
2.49

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I-002
503
2
2.30

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I-003
488
2
2.17

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I-004
488
2
2.20

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I-005
420
2
1.60

TABLE 11

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

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I-006
475
2
2.36

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I-007
503
2
2.61

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I-008
504
2
1.90

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I-009
479
2
2.80

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I-010
445
2
2.09

TABLE 12

Compound
MS
LC
LC/MS retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

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I-011
451
2
2.34

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I-012
431
2
2.26

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I-013
463
2
2.26

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I-014
471
2
2.70

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I-015
458
2
2.80

TABLE 13

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

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I-016
507
2
2.77

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I-017
452
2
2.03

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I-018
448
2
2.23

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I-019
487
2
2.47

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I-020
474
2
2.55

TABLE 14

Compound
MS
LC
LC/MS retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

I-021
451
2
2.31

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I-022
450
2
2.22

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I-023
449
2
2.19

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I-024
449
2
2.23

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I-025
451
2
2.25

TABLE 15

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

I-026
513
2
2.73

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I-027
497
2
2.10

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I-028
501
2
2.00

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I-029
499
2
2.20

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I-030
498
2
2.10

TABLE 16

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

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I-031
489
2
2.08

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I-032
498
2
2.10

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I-033
498
2
1.90

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I-034
493
2
1.60

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I-035
470
2
1.52

TABLE 17

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

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I-036
380
2
2.46

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I-037
408
2
2.69

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I-038
453
2
2.50

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I-039
458
2
2.60

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I-040
478
2
2.11

TABLE 18

Compound
MS

LC/MS

Chemical Structure
No.
{M + H]⁺
LC method
retention time (min)

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I-041
523
2
2.41

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I-042
495
2
2.52

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I-043
411
2
2.28

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I-044
408
1
2.50

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I-045
424
1
2.30

TABLE 19

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

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I-046
422
1
2.50

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I-047
466
1
2.50

embedded image

I-048
433
1
2.40

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I-049
449
1
2.40

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I-050
461
2
2.53

TABLE 20

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

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I-051
462
2
2.49

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I-052
412
1
2.26

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I-053
409
2
2.23

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I-054
396
1
2.10

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I-055
447
1
2.00

TABLE 21

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-056
463
1
2.10

embedded image

I-057
449
1
2.20

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I-058
463
1
1.80

embedded image

I-059
447
1
2.20

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I-060
395
2
1.51

TABLE 22

Com-
MS

LC/MS

pound
[M +
LC
retention

Chemical Structure
No.
H]⁺
method
time (min)

embedded image

I-061
395
2
1.43

embedded image

I-062
461
1
1.90

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I-063
445
2
2.52

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I-064
469
1
2.20

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I-065
384
2
2.40

TABLE 23

Com-
MS

LC/MS

pound
[M +
LC
retention

Chemical Structure
No.
H]⁺
method
time (min)

embedded image

I-066
413
1
2.10

embedded image

I-067
410
1
1.80

embedded image

I-068
428
1
1.80

embedded image

I-069
400
2
2.50

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I-070
446
1
2.00

TABLE 24

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-071
499
1
1.90

embedded image

I-072
447
1
2.20

embedded image

I-073
434
2
2.20

embedded image

I-074
378
2
2.00

embedded image

I-075
478
1
2.10

TABLE 25

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-076
461
2
2.27

embedded image

I-077
432
2
2.54

embedded image

I-078
448
2
2.65

embedded image

I-079
448
2
2.69

embedded image

I-080
478
1
2.10

TABLE 26

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-081
442
1
2.00

embedded image

I-082
479
1
1.90

embedded image

I-083
445
2
2.36

embedded image

I-084
385
1
1.91

embedded image

I-085
462
1
2.10

TABLE 27

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-086

2
2.05

embedded image

I-087
460
2
2.40

embedded image

I-088
478
1
1.90

embedded image

I-089
478
1
1.80

embedded image

I-090
477
1
1.90

TABLE 28

Com-
MS

LC/MS

pound
[M +
LC
retention

Chemical Structure
No.
H]⁺
method
time (min)

embedded image

I-091
431
1
2.30

embedded image

I-092
432
2
2.61

embedded image

I-093
433
2
1.19

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I-094
431
2
1.17

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I-095
465
2
2.14

TABLE 29

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-096
419
1
1.90

embedded image

I-097
448
2
2.20

embedded image

I-098
477
1
2.10

embedded image

I-099
465
2
1.80

embedded image

I-100
465
2
1.90

TABLE 30

Com-
MS

LC/MS

pound
[M +
LC
retention

Chemical Structure
No.
H]⁺
method
time (min)

embedded image

I-101
446
2
2.42

embedded image

I-102
432
2
1.98

embedded image

I-103
458
1
1.90

embedded image

I-104
435
2
1.96

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I-105
461
1
2.30

TABLE 31

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

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I-106
459
2
2.70

embedded image

I-107
446
2
2.21

embedded image

I-108
450
2
2.30

embedded image

I-109
434
2
2.16

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I-110
433
1
1.80

TABLE 32

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

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I-111
481
1
1.90

embedded image

I-112
435
2
2.00

embedded image

I-113
506
1
2.30

embedded image

I-114
506
1
2.30

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I-115
449
1
2.30

TABLE 33

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-116
449
1
2.20

embedded image

I-117
433
1
2.20

embedded image

I-118
433
1
2.10

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I-119
492
1
2.10

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I-120
492
1
2.00

TABLE 34

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-121
434
2
2.19

embedded image

I-122
450
2
2.36

embedded image

I-123
492
1
2.40

embedded image

I-124
492
1
2.30

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I-125
533
1
1.90

TABLE 35

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-126
533
1
1.90

embedded image

I-127
513
1
1.70

embedded image

I-128
492
1
2.10

embedded image

I-129
492
1
2.10

embedded image

I-130
456
1
2.20

TABLE 36

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-131
561
2
2.40

embedded image

I-132
476
1
2.30

embedded image

I-133
491
1
2.00

embedded image

I-134
477
1
1.80

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I-135
505
1
1.50

TABLE 37

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-136
505
1
1.90

embedded image

I-137
490
1
1.30

embedded image

I-138
493
1
2.20

embedded image

I-139
478
1
1.90

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I-140
418
1
1.20

TABLE 38

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-141
433
1
1.50

embedded image

I-142
417
1
1.40

embedded image

I-143
433
1
1.40

embedded image

I-144
476
1
1.67

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I-145
524
1
1.91

TABLE 39

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-146
490
1
1.81

embedded image

I-147
505
2
2.36

embedded image

I-148
519
2
2.39

embedded image

I-149
493
1
2.30

embedded image

I-150
457
1
2.10

TABLE 40

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-151
491
2
2.22

embedded image

I-152
509
2
1.94

embedded image

I-153
475
2
1.76

embedded image

I-154
461
2
2.10

embedded image

I-155
462
1
1.90

TABLE 41

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-156
476
1
2.20

embedded image

I-157
491
1
1.50

embedded image

I-158
491
1
1.55

embedded image

I-159
434
1
2.20

embedded image

I-160
464
2
2.27

TABLE 42

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]
LC method
retention time (min)

embedded image

I-161
478
2
2.56

embedded image

I-162
463
1
1.70

embedded image

I-163
464
1
1.60

embedded image

I-164
477
1
2.10

embedded image

I-165
463
1
1.80

TABLE 43

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-166
479
1
2.00

embedded image

I-167
510
1
1.79

embedded image

I-168
507
1
1.65

embedded image

I-169
479
2
2.45

embedded image

I-170
464
2
2.11

TABLE 44

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-171
443
1
1.80

embedded image

I-172
479
1
2.00

embedded image

I-173
463
1
1.90

embedded image

I-174
479
2
2.15

embedded image

I-175
479
2
2.18

TABLE 45

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-176
465
1
1.80

embedded image

I-177
465
1
1.60

embedded image

I-178
465
1
1.50

embedded image

I-179
450
1
1.50

embedded image

I-180
473
2
2.52

TABLE 46

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-181
521
1
1.79

embedded image

I-182
507
1
1.51

embedded image

I-183
459
1
2.11

embedded image

I-184
462
1
2.05

embedded image

I-185
478
1
1.90

TABLE 47

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-186
448
2
2.56

embedded image

I-187
435
1
2.10

embedded image

I-188
491
1
2.00

embedded image

I-189
477
1
1.80

embedded image

I-190
448
2
2.15

TABLE 48

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-191
449
2
1.87

embedded image

I-192
482
2
2.84

embedded image

I-193
462
2
2.80

embedded image

I-194
449
1
1.53

embedded image

I-195
479
1
1.80

TABLE 49

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-196
476
2
2.52

embedded image

I-197
462
2
2.83

embedded image

I-198
418
1
2.16

embedded image

I-199
492
1
1.90

embedded image

I-200
478
1
1.80

TABLE 50

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-201
462
1
2.14

embedded image

I-202
418
1
2.17

embedded image

I-203
418
1
2.17

embedded image

I-204
432
2
2.45

embedded image

I-205
431
2
2.48

TABLE 51

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-206
434
2
2.58

embedded image

I-207
434
2
2.58

embedded image

I-208
462
1
2.14

embedded image

I-209
462
1
2.14

embedded image

I-210
462
2
2.87

TABLE 52

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-211
458
2
2.38

embedded image

I-212
475
1
1.90

embedded image

I-213
464
1
2.29

embedded image

I-214
434
2
2.57

embedded image

I-215
448
2
2.59

TABLE 53

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-216
400
2
2.47

embedded image

I-217
502
2
2.22

embedded image

I-218
432
1
2.20

embedded image

I-219
405
2
2.28

embedded image

I-220
492
2
1.84

TABLE 54

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-221
464
2
2.61

embedded image

I-222
478
1
2.26

embedded image

I-223
464
1
2.04

embedded image

I-224
418
2
2.51

embedded image

I-225
448
2
2.21

TABLE 55

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-226
478
1
2.29

embedded image

I-227
464
1
2.32

embedded image

I-228
479
1
2.15

embedded image

I-229
465
1
1.87

embedded image

I-230
448
2
2.51

TABLE 56

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-231
462
2
2.47

embedded image

I-232
448
1
2.18

embedded image

I-233
449
2
2.00

embedded image

I-234
462
1
1.99

embedded image

I-235
452
2
2.67

TABLE 57

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-236
448
2
2.66

embedded image

I-237
449
2
2.38

embedded image

I-238
492
2
2.51

embedded image

I-239
448
1
2.37

embedded image

I-240
450
1
2.09

TABLE 58

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-241
464
1
2.03

embedded image

I-242
477
1
2.39

embedded image

I-243
477
2
2.05

embedded image

I-244
428
1
2.12

embedded image

I-245
475
1
2.10

TABLE 59

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-246
421
2
1.87

embedded image

I-247
462
1
2.28

embedded image

I-248
493
1
2.19

embedded image

I-249
478
1
2.38

embedded image

I-250
478
1
2.09

TABLE 60

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-251
492
1
2.37

embedded image

I-252
462
1
2.39

embedded image

I-253
434
1
1.41

embedded image

I-254
448
2
2.59

embedded image

I-255
448
2
2.59

TABLE 61

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-256
478
1
2.14

embedded image

I-257
448
1
2.39

embedded image

I-258
478
1
2.16

embedded image

I-259
448
1
2.42

embedded image

I-260
438
2
2.33

TABLE 62

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-261
492
2
2.70

embedded image

I-262
478
2
2.71

embedded image

I-263
492
2
2.73

embedded image

I-264
478
2
2.75

embedded image

I-265
462
2
2.73

TABLE 63

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-266
462
2
2.76

embedded image

I-267
493
2
2.60

embedded image

I-268
493
2
2.56

embedded image

I-269
408
2
2.42

embedded image

I-270
431
2
2.49

TABLE 64

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-271
478
1
2.02

embedded image

I-272
464
1
1.73

embedded image

I-273
492
1
2.15

embedded image

I-274
478
1
1.85

embedded image

I-275
478
1
1.97

TABLE 65

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-276
492
1
2.12

embedded image

I-277
464
1
1.72

embedded image

I-278
478
1
1.86

embedded image

I-279
448
2
2.68

embedded image

I-280
448
2
2.67

TABLE 66

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-281
492
1
2.30

embedded image

I-282
442
1
2.37

embedded image

I-283
448
1
2.40

embedded image

I-284
434
2
2.50

embedded image

I-285
434
2
2.50

TABLE 67

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-286
478
2
2.45

embedded image

I-287
442
1
2.10

embedded image

I-288
507
1
2.04

embedded image

I-289
488
2
2.63

embedded image

I-290
484
1
2.44

TABLE 68

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-291
449
2
2.51

embedded image

I-292
486
2
2.72

embedded image

I-293
476
2
2.87

embedded image

I-294
434
1
1.99

embedded image

I-295
477
1
2.18

TABLE 69

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-296
430
1
2.07

embedded image

I-297
473
1
2.11

embedded image

I-298
463
1
1.96

embedded image

I-299
462
1
2.48

embedded image

I-300
472
1
2.33

TABLE 70

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-301
470
1
2.35

embedded image

I-302
488
1
2.39

embedded image

I-303
476
1
2.54

embedded image

I-304
506
1
2.53

embedded image

I-305
492
1
2.51

TABLE 71

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-306
461
1
2.27

embedded image

I-307
469
1
2.17

embedded image

I-308
487
1
2.21

embedded image

I-309
477
1
2.09

embedded image

I-310
448
2
2.29

TABLE 72

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-311
464
2
2.28

embedded image

I-312
462
2
2.49

embedded image

I-313
470
2
2.34

embedded image

I-314
488
2
2.43

embedded image

I-315
462
2
2.42

TABLE 73

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-316
478
2
2.40

embedded image

I-317
476
2
2.61

embedded image

I-318
484
2
2.45

embedded image

I-319
502
2
2.54

embedded image

I-320
449
2
2.53

TABLE 74

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-321
484
2
2.73

embedded image

I-322
502
2
2.80

embedded image

I-323
463
1
1.83

embedded image

I-324
463
1
1.69

embedded image

I-325
452
1
2.27

TABLE 75

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-326
466
1
2.40

embedded image

I-327
462
1
2.52

embedded image

I-328
492
1
2.27

embedded image

I-329
476
1
2.74

embedded image

I-330
502
1
2.51

TABLE 76

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-331
488
2
2.61

embedded image

I-332
449
1
2.26

embedded image

I-333
484
1
2.50

embedded image

I-334
502
1
2.55

embedded image

I-335
512
2
2.36

TABLE 77

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-336
463
1
2.40

embedded image

I-337
498
1
2.56

embedded image

I-338
516
1
2.67

embedded image

I-339
447
2
2.47

embedded image

I-340
433
1
2.10

TABLE 78

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-341
483
2
2.53

embedded image

I-342
468
1
2.30

embedded image

I-343
486
1
2.40

embedded image

I-344
501
2
2.59

embedded image

I-345
477
2
2.19

TABLE 79

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-346
491
2
2.46

embedded image

I-347
446
1
2.25

embedded image

I-348
476
1
2.21

embedded image

I-349
462
1
2.26

embedded image

I-350
462
1
1.98

TABLE 80

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-351
432
1
2.27

embedded image

I-352
437
1
1.92

embedded image

I-353
433
1
2.09

embedded image

I-354
432
2
2.53

embedded image

I-355
446
2
2.64

TABLE 81

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-356
462
2
2.67

embedded image

I-357
477
1
2.16

embedded image

I-358
468
1
2.41

embedded image

I-359
486
1
2.46

embedded image

I-360
491
1
2.29

TABLE 82

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-361
482
1
2.47

embedded image

I-362
500
1
2.56

embedded image

I-363
496
1
2.26

embedded image

I-364
510
1
2.39

embedded image

I-365
510
1
2.11

TABLE 83

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-366
492
1
2.12

embedded image

I-367
480
1
2.15

embedded image

I-368
494
1
2.27

embedded image

I-369
496
1
2.00

embedded image

I-370
475
1
2.38

TABLE 84

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-371
463
2
2.67

embedded image

I-372
492
2
2.81

embedded image

I-373
490
2
2.97

embedded image

I-374
492
2
2.51

embedded image

I-375
506
2
2.79

TABLE 85

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-376
476
2
2.83

embedded image

I-377
498
1
2.52

embedded image

I-378
516
1
2.61

embedded image

I-379
462
1
2.52

embedded image

I-380
460
1
2.48

TABLE 86

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-381
490
1
2.40

embedded image

I-382
476
1
2.45

embedded image

I-383
446
1
2.43

embedded image

I-384
476
1
2.18

embedded image

I-385
437
1
1.91

TABLE 87

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-386
476
2
2.32

embedded image

I-387
433
2
2.18

embedded image

I-388
477
2
2.17

embedded image

I-389
447
2
2.19

embedded image

I-390
447
2
2.30

TABLE 88

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-391
491
2
2.32

embedded image

I-392
461
2
2.35

embedded image

I-393
462
1
2.47

embedded image

I-394
448
1
2.29

embedded image

I-395
479
1
2.11

TABLE 89

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-396
460
1
2.52

embedded image

I-397
473
1
2.17

embedded image

I-398
474
1
2.65

embedded image

I-399
487
1
2.25

embedded image

I-400
476
1
2.61

TABLE 90

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-401
489
1
2.27

embedded image

I-402
490
1
2.70

embedded image

I-403
513
2
2.00

embedded image

I-404
503
2
2.64

embedded image

I-405
489
2
2.51

TABLE 91

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

I-406
503
1
2.38

embedded image

I-407
476
2
2.67

embedded image

I-408
460
1
2.44

embedded image

I-409
489
2
2.53

embedded image

I-410
495
1
1.97

TABLE 92

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

I-411
476
1
2.09

embedded image

I-412
451
1
2.00

embedded image

I-413
479
1
2.21

embedded image

I-414
465
1
2.02

embedded image

I-415
545
1
2.58

TABLE 93

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

I-416
435
2
2.27

embedded image

I-417
479
2
2.27

embedded image

I-418
449
2
2.28

embedded image

I-419
476
2
2.89

embedded image

I-420
449
2
2.39

TABLE 94

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

I-421
493
2
2.40

embedded image

I-422
463
2
2.41

embedded image

I-423
449
2
2.41

embedded image

I-424
493
2
2.39

embedded image

I-425
463
2
2.42

TABLE 95

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

I-426
463
2
2.53

embedded image

I-427
507
2
2.52

embedded image

I-428
477
2
2.55

embedded image

I-429
478
1
2.00

embedded image

I-430
473
1
2.08

TABLE 96

LC/MS

Chemical
Compound
MS
LC
retention

Structure
No.
[M + H]⁺
method
time (min)

embedded image

I-431
462
1
2.26

embedded image

I-432
462
1
1.97

embedded image

I-433
479
1
2.08

embedded image

I-434
413
2
2.52

embedded image

I-435
456
2
2.48

TABLE 97

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

I-436
440
2
2.71

embedded image

I-437
426
2
2.55

embedded image

I-438
450
2
2.91

embedded image

I-439
488
2
2.85

embedded image

I-440
463
1
2.32

TABLE 98

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

I-441
449
1
2.18

embedded image

I-442
503
1
2.37

embedded image

I-443
489
1
2.26

embedded image

I-444
478
1
1.75

embedded image

I-445
492
1
1.84

TABLE 99

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

I-446
510
1
2.50

embedded image

I-447
494
1
2.69

embedded image

I-448
480
1
2.51

embedded image

I-449
476
1
2.62

embedded image

I-450
461
1
2.31

TABLE 100

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

I-451
476
1
2.38

embedded image

I-452
452
1
2.23

embedded image

I-453
466
1
2.41

embedded image

I-454
450
1
2.30

embedded image

I-455
462
2
2.72

TABLE 101

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

I-456
508
2
2.12

embedded image

I-457
433
2
2.36

embedded image

I-458
447
2
2.39

embedded image

I-459
449
1
2.44

embedded image

I-460
469
2
2.04

TABLE 102

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

I-461
483
2
2.04

embedded image

I-462
463
2
2.61

embedded image

I-463
507
2
2.64

embedded image

I-464
449
1
2.19

embedded image

I-465
492
2
2.73

TABLE 103

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

I-466
503
2
2.61

embedded image

I-467
468
2
2.38

embedded image

I-468
440
2
2.23

embedded image

I-469
497
2
2.88

embedded image

I-470
520
2
2.70

TABLE 104

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

I-471
491
1
2.24

embedded image

I-472
493
2
2.60

embedded image

I-473
398
2
2.38

embedded image

I-474
426
2
2.61

embedded image

I-475
442
2
2.36

TABLE 105

LC/MS

Compound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

I-476
442
2
2.12

embedded image

I-477
412
2
2.39

embedded image

I-478
477
1
1.89

embedded image

I-479
461
1
2.39

embedded image

I-480
497
2
2.32

TABLE 106

Compound
MS
LC
LC/MS

Chemical Structure
No.
[M + H]⁺
method
retention time (min)

embedded image

I-481
477
2
2.35

embedded image

I-482
465
2
2.41

embedded image

I-483
463
1
1.89

embedded image

I-484
456
2
2.47

embedded image

I-485
443
2
2.24

TABLE 107

Compound
MS
LC
LC/MS

Chemical Structure
No.
[M + H]⁺
method
retention time (min)

embedded image

I-486
487
1
2.28

embedded image

I-487
489
1
1.97

embedded image

I-488
503
1
2.07

embedded image

I-489
492
1
2.32

embedded image

I-490
506
1
2.39

TABLE 108

Compound
MS
LC
LC/MS

Chemical Structure
No.
[M + H]⁺
method
retention time (min)

embedded image

I-491
492
1
2.06

embedded image

I-492
506
1
2.15

embedded image

I-493
487
1
1.98

embedded image

I-494
503
2
2.65

embedded image

I-495
487
2
2.59

TABLE 109

Compound
MS
LC
LC/MS

Chemical Structure
No.
[M + H]⁺
method
retention time (min)

embedded image

I-496
531
2
2.63

embedded image

I-497
547
2
2.70

embedded image

I-498
522
2
2.23

embedded image

I-499
480
2
2.44

embedded image

I-500
520
2
2.63

TABLE 110

Compound
MS
LC
LC/MS

Chemical Structure
No.
[M + H]⁺
method
retention time (min)

embedded image

I-501
506
2
2.24

embedded image

I-502
504
1
1.96

embedded image

I-503
487
1
2.34

embedded image

I-504
519
1
2.39

embedded image

I-505
545
2
2.61

TABLE 111

Compound
MS
LC
LC/MS

Chemical Structure
No.
[M + H]⁺
method
retention time (min)

embedded image

I-506
529
2
2.55

embedded image

I-507
496
2
2.45

embedded image

I-508
459
2
2.11

embedded image

I-509
423
2
2.20

embedded image

I-510
474
2
2.21

TABLE 112

Compound
MS
LC
LC/MS

Chemical Structure
No.
[M + H]⁺
method
retention time (min)

embedded image

I-511
437
2
2.29

embedded image

I-512
473
1
2.36

embedded image

I-513
487
1
2.49

embedded image

I-514
501
1
2.24

embedded image

I-515
475
1
2.38

TABLE 113

Compound
MS
LC
LC/MS

Chemical Structure
No.
[M + H]⁺
method
retention time (min)

embedded image

I-516
474
1
2.43

embedded image

I-517
505
1
2.26

embedded image

I-518
488
1
2.39

embedded image

I-519
502
1
2.55

embedded image

I-520
476
1
1.70

TABLE 114

Compound
MS
LC
LC/MS

Chemical Structure
No.
[M + H]⁺
method
retention time (min)

embedded image

I-521
490
1
1.96

embedded image

I-522
491
1
1.71

embedded image

I-523
505
1
1.98

embedded image

I-524
490
1
1.65

embedded image

I-525
490
1
1.91

TABLE 115

Compound
MS
LC
LC/MS

Chemical Structure
No.
[M + H]⁺
method
retention time (min)

embedded image

I-526
529
2
2.43

embedded image

I-527
432
1
2.46

embedded image

I-528
434
1
2.50

embedded image

I-529
477
1
1.76

embedded image

I-530
504
1
2.30

TABLE 116

Compound
MS
LC
LC/MS

Chemical Structure
No.
[M + H]⁺
method
retention time (min)

embedded image

I-531
436
2
2.28

embedded image

I-532
480
2
2.25

embedded image

I-533
464
2
2.51

embedded image

I-534
515
1
1.75

embedded image

I-535
487
1
1.89

TABLE 117

Compound
MS
LC
LC/MS

Chemical Structure
No.
[M + H]⁺
method
retention time (min)

embedded image

I-536
473
1
1.80

embedded image

I-537
501
2
2.25

embedded image

I-538
515
2
2.31

embedded image

I-539
476
1
2.27

embedded image

I-540
461
1
2.23

TABLE 118

Compound
MS
LC
LC/MS

Chemical Structure
No.
[M + H]⁺
method
retention time (min)

embedded image

I-541
476
1
2.51

embedded image

I-542
478
1
2.12

embedded image

I-543
463
1
2.09

embedded image

I-544
478
1
2.37

embedded image

I-545
478
1
2.14

TABLE 119

Compound
MS
LC
LC/MS

Chemical Structure
No.
[M + H]⁺
method
retention time (min)

embedded image

I-546
531
2
2.52

embedded image

I-547
533
2
2.53

embedded image

I-548
480
2
2.38

embedded image

I-549
515
2
2.44

embedded image

I-550
457
2
2.22

TABLE 120

Compound
MS
LC
LC/MS

Chemical Structure
No.
[M + H]⁺
method
retention time (min)

embedded image

I-551
506
2
2.39

embedded image

I-552
476
1
2.32

embedded image

I-553
471
2
2.37

embedded image

I-554
418
2
2.08

embedded image

I-555
433
2
2.11

TABLE 121

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-556
506
2
2.43

embedded image

I-557
492
2
2.19

embedded image

I-558
450
2
2.53

embedded image

I-559
464
2
2.65

embedded image

I-560
510
2
2.35

TABLE 122

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-561
495
2
2.31

embedded image

I-562
479
2
2.19

embedded image

I-563
514
2
2.20

embedded image

I-564
479
1
1.83

embedded image

I-565
493
1
2.14

TABLE 123

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-566
463
1
1.72

embedded image

I-567
477
1
2.02

embedded image

I-568
493
2
2.21

embedded image

I-569
507
2
2.54

embedded image

I-570
493
2
2.19

TABLE 124

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-571
507
2
2.51

embedded image

I-572
476
3
3.28

embedded image

I-573
490
3
3.35

embedded image

I-574
504
3
3.32

embedded image

I-575
518
3
3.41

TABLE 125

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-576
519
3
3.40

embedded image

I-577
515
3
3.24

embedded image

I-578
518
3
3.68

embedded image

I-579
530
3
3.45

embedded image

I-580
546
3
3.40

TABLE 126

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-581
534
3
3.50

embedded image

I-582
548
3
3.37

embedded image

I-583
547
3
2.43

embedded image

I-584
519
2
2.17

embedded image

I-585
503
2
2.10

TABLE 127

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-586
517
2
2.39

embedded image

I-587
487
2
2.24

embedded image

I-588
459
1
2.20

embedded image

I-589
438
1
2.34

embedded image

I-590
503
1
2.01

TABLE 128

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-591
482
1
2.15

embedded image

I-592
475
1
1.52

embedded image

I-593
489
1
1.60

embedded image

I-594
517
1
1.83

embedded image

I-595
503
1
1.75

TABLE 129

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

I-596
487
2
1.82

embedded image

I-598
501
2
2.27

embedded image

I-598
501
2
2.27

TABLE 130

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-001
404
1
2.30

embedded image

II-002
420
1
2.10

embedded image

II-003
418
1
2.40

embedded image

II-004
462
1
2.40

embedded image

II-005
459
1
1.90

TABLE 131

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-006
443
1
1.80

embedded image

II-007
409
1
1.90

embedded image

II-008
406
1
1.50

embedded image

II-009
424
1
1.70

embedded image

II-010
466
1
1.90

TABLE 132

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-011
421
1
1.30

embedded image

II-012
474
1
2.00

embedded image

II-013
438
1
1.80

embedded image

II-014
475
1
1.70

embedded image

II-015
473
1
1.70

TABLE 133

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-016
474
1
1.70

embedded image

II-017
474
1
1.70

embedded image

II-018
473
1
1.90

embedded image

II-019
457
1
2.10

embedded image

II-020
502
1
2.10

TABLE 134

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-021
502
1
2.10

embedded image

II-022
488
1
1.80

embedded image

II-023
488
1
1.80

embedded image

II-024
488
1
1.90

embedded image

II-025
488
1
1.90

TABLE 135

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-026
452
1
2.00

embedded image

II-027
472
1
2.10

embedded image

II-028
487
1
1.80

embedded image

II-029
473
1
1.60

embedded image

II-030
486
1
1.20

TABLE 136

LC/MS

Com-
MS
LC
retention

pound
[M +
meth-
time

Chemical Structure
No.
H]⁺
od
(min)

embedded image

II-031
501
1
1.50

embedded image

II-032
489
1
2.00

embedded image

II-033
474
1
1.70

embedded image

II-034
453
1
1.80

embedded image

II-035
489
1
2.10

TABLE 137

LC/MS

Com-
MS
LC
retention

pound
[M +
meth-
time

Chemical Structure
No.
H]⁺
od
(min)

embedded image

II-036
460
1
1.50

embedded image

II-037
473
1
2.00

embedded image

II-038
473
1
1.90

embedded image

II-039
475
1
1.80

embedded image

II-040
439
1
1.60

Table 138

LC/MS

reten-

Com-
MS
LC
tion

pound
[M +
meth-
time

Chemical Structure
No.
H]⁺
od
(min)

embedded image

II-041
459
1
1.70

embedded image

II-042
475
1
1.80

embedded image

II-043
459
1
1.70

embedded image

II-044
446
1
1.40

embedded image

II-045
461
1
1.70

TABLE 139

LC/MS

reten-

Com-
MS
LC
tion

pound
[M +
meth-
time

Chemical Structure
No.
H]⁺
od
(min)

embedded image

II-046
461
1
1.40

embedded image

II-047
474
1
1.80

embedded image

II-048
431
1
2.00

embedded image

II-049
487
1
1.80

embedded image

II-050
473
1
1.70

TABLE 140

LC/MS

Com-
MS
LC
retention

pound
[M +
meth-
time

Chemical Structure
No.
H]⁺
od
(min)

embedded image

II-051
488
1
1.60

embedded image

II-052
475
1
1.70

embedded image

II-053
488
1
1.70

embedded image

II-054
474
1
1.60

embedded image

II-055
427
2
2.13

TABLE 141

LC/MS

Com-
MS
LC
retention

pound
[M +
meth-
time

Chemical Structure
No.
H]⁺
od
(min)

embedded image

II-056
509
1
2.43

embedded image

II-057
434
1
2.09

embedded image

II-058
416
1
1.23

embedded image

II-059
447
1
1.93

embedded image

II-060
459
2
2.07

TABLE 142

LC/MS

reten-

Com-

LC
tion

pound
MS
meth-
time

Chemical Structure
No.
[M + H]⁺
od
(min)

embedded image

II-061
483
2
2.23

embedded image

II-062
447
2
2.08

embedded image

II-063
447
1
1.9

embedded image

II-064
485
1
1.76

embedded image

II-065
466
1
1.36

TABLE 143

LC/MS

Com-

retention

pound
MS
LC
time

Chemical Structure
No.
[M + H]⁺
method
(min)

embedded image

II-066
426
1
2.47

embedded image

II-067
416
1
2.43

embedded image

II-068
457
1
1.93

embedded image

II-069
458
1
1.88

embedded image

II-070
440
1
1.68

TABLE 144

LC/MS

Com-

retention

pound
MS
LC
time

Chemical Structure
No.
[M + H]⁺
method
(min)

embedded image

II-071
424
1
1.49

embedded image

II-072
419
1
1.25

embedded image

II-073
443
1
2.03

embedded image

II-074
431
1
1.55

embedded image

II-075
472
1
1.48

TABLE 145

LC/MS

Com-

reten-

pound
MS
LC
tion

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

II-076
520
1
1.76

embedded image

II-077
486
1
1.55

embedded image

II-078
487
1
1.39

embedded image

II-079
430
1
1.91

embedded image

II-080
506
1
1.69

TABLE 146

LC/MS

Com-

retention

pound
MS
LC
time

Chemical Structure
No.
[M + H]⁺
method
(min)

embedded image

II-081
415
1
1.96

embedded image

II-082
471
1
1.78

embedded image

II-083
428
1
2.09

embedded image

II-084
457
1
1.23

embedded image

II-085
457
1
1.72

TABLE 147

LC/MS

Com-

retention

pound
MS
LC
time

Chemical Structure
No.
[M + H]⁺
method
(min)

embedded image

II-086
430
1
1.79

embedded image

II-087
458
1
1.58

embedded image

II-088
493
1
1.76

embedded image

II-089
444
1
1.77

embedded image

II-090
443
1
1.62

TABLE 148

LC/MS

Com-

retention

pound
MS
LC
time

Chemical Structure
No.
[M + H]⁺
method
(min)

embedded image

II-091
487
1
1.55

embedded image

II-092
457
1
1.74

embedded image

II-093
471
1
1.86

embedded image

II-094
458
1
1.75

embedded image

II-095
473
1
1.87

TABLE 149

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-096
425
1
2.30

embedded image

II-097
446
1
2.20

embedded image

II-098
392
1
1.90

embedded image

II-099
445
1
2.00

embedded image

II-100
459
1
1.60

TABLE 150

Com-

LC/MS

pound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

II-101
443
1
2.00

embedded image

II-102
465
1
1.90

embedded image

II-103
495
1
1.60

embedded image

II-104
474
1
1.90

embedded image

II-105
458
1
1.90

TABLE 151

Com-

LC/MS

pound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

II-106
427
1
2.40

embedded image

II-107
415
1
1.60

embedded image

II-108
454
1
1.70

embedded image

II-109
461
1
1.70

embedded image

II-110
461
1
1.80

TABLE 152

Com-

LC/MS

pound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

II-111
445
1
1.70

embedded image

II-112
477
1
1.60

embedded image

II-113
429
1
1.60

embedded image

II-114
488
1
2.20

embedded image

II-115
488
1
2.20

TABLE 153

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-116
509
1
1.70

embedded image

II-117
529
1
1.90

embedded image

II-118
529
1
2.00

embedded image

II-119
442
1
2.00

embedded image

II-120
414
1
1.10

TABLE 154

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-121
429
1
1.50

embedded image

II-122
413
1
1.40

embedded image

II-123
429
1
1.50

embedded image

II-124
458
1
1.60

embedded image

II-125
472
1
1.80

TABLE 155

Com-

LC/MS

pound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

II-126
459
1
1.70

embedded image

II-127
455
1
1.95

embedded image

II-128
517
1
1.72

embedded image

II-129
503
1
1.48

embedded image

II-130
504
1
1.88

TABLE 156

Com-

LC/MS

pound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

II-131
458
1
1.81

embedded image

II-132
489
1
1.56

embedded image

II-133
445
1
1.67

embedded image

II-134
391
2
1.37

embedded image

II-135
391
2
1.31

TABLE 157

Com-

LC/MS

pound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

II-136
459
2
1.90

embedded image

II-137
460
2
1.90

embedded image

II-138
460
2
1.90

embedded image

II-139
435
2
2.20

embedded image

II-140
465
2
2.10

TABLE 158

Com-
MS

LC/MS

pound
[M +
LC
retention

Chemical Structure
No.
H]⁺
method
time (min)

embedded image

II-141
461
2
1.90

embedded image

II-142
465
2
2.20

embedded image

II-143
419
2
2.10

embedded image

II-144
432
2
1.90

embedded image

II-145
473
2
1.70

TABLE 159

Com-
MS

LC/MS

pound
[M +
LC
retention

Chemical Structure
No.
H]⁺
method
time (min)

embedded image

II-146
458
2
1.98

embedded image

II-147
486
2
1.96

embedded image

II-148
441
2
2.07

embedded image

II-149
413
2
1.85

embedded image

II-150
406
2
1.88

TABLE 160

Com-

LC/MS

pound
MS
LC
retention

Chemical Structure
No.
[M + H]⁺
method
time (min)

embedded image

II-151
420
2
2.03

embedded image

II-152
433
2
1.97

embedded image

II-153
419
2
1.79

embedded image

II-154
449
2
1.97

embedded image

II-155
404
2
2.07

TABLE 161

Com
MS

LC/MS

pound
[M +
LC
retention

Chemical Structure
No.
H]⁺
method
time (min)

embedded image

II-156
433
2
2.40

embedded image

II-157
458
2
1.77

embedded image

II-158
486
2
1.21

embedded image

II-159
472
2
1.20

embedded image

II-160
420
2
2.41

TABLE 162

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-161
449
2
1.88

embedded image

II-162
406
2
1.57

embedded image

II-163
474
2
2.16

embedded image

II-164
431
2
1.86

embedded image

II-165
474
2
2.13

TABLE 163

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-166
515
2
2.19

embedded image

II-167
501
2
2.12

embedded image

II-168
505
2
1.76

embedded image

II-169
487
2
2.03

embedded image

II-170
487
2
2.06

TABLE 164

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-171
551
2
2.23

embedded image

II-172
501
2
2.19

embedded image

II-173
469
2
2.39

embedded image

II-174
512
2
2.40

embedded image

II-175
498
2
2.05

TABLE 165

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-176
501
2
2.10

embedded image

II-177
428
2
1.97

embedded image

II-178
454
2
2.42

embedded image

II-179
432
2
2.10

embedded image

II-180
459
2
2.15

TABLE 166

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-181
445
2
2.14

embedded image

II-182
418
2
2.13

embedded image

II-183
396
2
2.30

embedded image

II-184
488
2
2.27

embedded image

II-185
488
2
1.79

TABLE 167

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-186
473
2
2.23

embedded image

II-187
421
2
1.92

embedded image

II-188
430
2
2.25

embedded image

II-189
459
2
2.40

embedded image

II-190
413
2
2.70

TABLE 168

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-191
444
2
2.06

embedded image

II-192
448
2
1.83

embedded image

II-193
446
2
2.06

embedded image

II-194
445
2
2.04

embedded image

II-195
445
2
2.08

TABLE 169

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-196
376
2
2.17

embedded image

II-197
404
2
2.43

embedded image

II-198
519
2
2.34

embedded image

II-199
491
2
2.37

embedded image

II-200
407
2
2.22

TABLE 170

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-201
408
2
2.35

embedded image

II-202
405
2
1.94

embedded image

II-203
428
2
2.40

embedded image

II-204
444
2
2.50

embedded image

II-205
441
2
2.40

TABLE 171

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-206
442
2
2.00

embedded image

II-207
583
2
3.30

embedded image

II-208
438
2
2.50

embedded image

II-209
429
2
2.10

embedded image

II-210
442
2
2.30

TABLE 172

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-211
540
2
3.10

embedded image

II-212
441
2
2.40

embedded image

II-213
444
2
2.60

embedded image

II-214
362
2
2.20

embedded image

II-215
444
2
2.10

TABLE 173

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-216
457
2
2.10

embedded image

II-217
460
2
2.20

embedded image

II-218
460
2
2.20

embedded image

II-219
444
2
2.00

embedded image

II-220
429
2
2.20

TABLE 174

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-221
380
2
2.20

embedded image

II-222
396
2
2.30

embedded image

II-223
445
2
2.40

embedded image

II-224
445
2
2.40

embedded image

II-225
430
2
2.20

TABLE 175

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-226
445
2
1.80

embedded image

II-227
445
2
1.80

embedded image

II-228
483
2
2.40

embedded image

II-229
498
2
2.20

embedded image

II-230
524
2
1.40

TABLE 176

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-231
444
2
2.00

embedded image

II-232
443
2
1.70

embedded image

II-233
401
2
2.12

embedded image

II-234
431
2
1.85

embedded image

II-235
460
2
2.50

TABLE 177

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-236
490
2
1.88

embedded image

II-237
487
2
2.07

embedded image

II-238
448
2
2.56

embedded image

II-239
444
2
2.55

embedded image

II-240
445
2
2.24

TABLE 178

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-241
488
2
2.39

embedded image

II-242
473
2
1.93

embedded image

II-243
460
2
2.18

embedded image

II-244
473
2
2.51

embedded image

II-245
522
2
2.12

TABLE 179

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-246
441
2
2.46

embedded image

II-247
429
2
2.37

embedded image

II-248
445
2
2.52

embedded image

II-249
457
2
2.09

embedded image

II-250
445
2
1.98

TABLE 180

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-251
461
2
1.18

embedded image

II-252
441
2
2.20

embedded image

II-253
429
2
1.90

embedded image

II-254
445
2
2.06

embedded image

II-255
445
2
2.13

TABLE 181

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-256
445
2
2.55

embedded image

II-257
429
2
2.44

embedded image

II-258
461
2
1.56

embedded image

II-259
442
2
2.39

embedded image

II-260
446
2
2.47

TABLE 182

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-261
430
2
2.25

embedded image

II-262
446
2
2.41

embedded image

II-263
430
2
2.36

embedded image

II-264
461
2
2.20

embedded image

II-265
445
2
2.09

TABLE 183

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-266
476
2
1.93

embedded image

II-267
442
2
2.05

embedded image

II-268
446
2
2.09

embedded image

II-269
430
2
1.94

embedded image

II-270
446
2
2.20

TABLE 184

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-271
430
2
2.03

embedded image

II-272
478
2
2.70

embedded image

II-273
458
2
2.65

embedded image

II-274
458
2
2.68

embedded image

II-275
458
2
2.74

TABLE 185

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-276
461
2
1.60

embedded image

II-277
503
2
1.98

embedded image

II-278
475
2
2.29

embedded image

II-279
460
2
1.94

embedded image

II-280
475
2
1.98

TABLE 186

Compound
MS

LC/MS

Chemical Structure
No.
[M + H]⁺
LC method
retention time (min)

embedded image

II-281
475
2
2.03

Test Examples

Stably expressing cell line (C6BU-1 cell transfected with human P2X₃receptor gene (GenBank accession number Y07683)) was used. The cells were seeded in a 96-well microtiter plate at a concentration of 8000 cells/well and cultured in the medium (8.3% fetal bovine serum, 8.3% horse serum, 1% antibiotic and antifungal in DMEM) for one day at 37° C. under 5% carbon dioxide atmosphere. The medium was replaced with 4 μM Fluo-3-AM solution (pH7.5) containing 20 mM HEPES, 137 mM NaCl, 2.7 mM KCl, 0.9 mM MgCl₂, 5.0 mM CaCl₂, 5.6 mM D-glucose, 2.5 mM probenecid, 10% BSA, and 0.08% Pluronic F-127, and incubated at 37° C. under 5% dioxide carbon atmosphere for one hour. The plate was washed with washing buffer (20 mM HEPES, 137 mM NaCl, 2.7 mM KCl, 0.9 mM MgCl₂, 5.0 mM CaCl₂, 5.6 mM D-glucose, 2.5 mM probenecid, pH7.5), and each well was added with 40 μL of this buffer. The plate was placed in High-Throughput Screening System FDSS 3000 (Hamamatsu Photonics K.K.). Measurement of fluorescence intensity by FDSS 3000 was started, and 40 p. 1.4 of DMSO solutions containing different concentrations of the test compound as prepared by dilution with dilution buffer (20 mM HEPES, 137 mM NaCl, 2.7 mM KCl, 0.9 mM MgCl₂, 5.0 mM CaCl₂, 5.6 mM D-glucose, 2.5 mM probenecid, 0.1% Pluronic F-127, pH7.5) were dispensed to each well through the built-in automatic dispenser. Five minutes after, 40 nM ATP solution (50 μL) prepared by dilution with the dilution buffer was dispensed through the built-in automatic dispenser, and the measurement of fluorescence intensity was continued for 3 min. For each well, the specific maximum fluorescence intensity was calculated as the ratio of the maximum fluorescence intensity after addition of the ATP solution to the fluorescence intensity at the starting of the measurement. The 50% inhibitory concentration (IC₅₀) was calculated under the assumption that the specific maximum fluorescence intensity without test compound is 0% inhibition and that the specific maximum fluorescence intensity when the dilution buffer was added in place of ATP solution is 100% inhibition, to evaluate the inhibitory activity of the test compound. FDSS software (Hamamatsu Photonics K.K.) was used for calculation of the specific maximum fluorescence intensity. 1050 was calculated using Microsoft™ Excel™ (Microsoft Corporation) and XLfit™ (ID Business Solutions Ltd.).

The results of the compounds of the invention are shown in the following tables.

TABLE 187

Compound
P2X3

No.
IC50 (μM)

I-001
0.032

I-002
0.024

I-003
0.040

I-004
0.012

I-005
0.247

I-006
0.027

I-007
0.100

I-008
0.014

I-009
0.014

I-010
0.595

I-011
0.270

I-012
0.340

I-014
0.134

I-015
0.012

I-016
0.079

I-019
0.132

I-020
0.021

I-021
0.382

I-026
0.339

I-027
0.040

I-028
0.075

I-029
0.160

I-030
0.053

I-031
0.700

I-032
0.160

I-033
0.053

I-034
0.700

I-037
0.954

I-038
0.926

I-039
0.012

I-044
0.468

I-046
0.580

I-047
0.221

I-048
0.752

I-050
0.642

I-051
0.277

I-052
0.187

I-055
0.596

I-057
0.159

I-058
0.082

I-059
0.260

I-064
0.137

I-066
0.434

I-068
0.305

I-070
0.519

I-072
0.352

I-075
0.013

I-077
0.048

I-078
0.016

I-225
0.065

I-226
0.012

I-227
0.008

I-228
0.015

I-229
0.029

I-230
0.018

I-231
0.023

I-232
0.024

I-233
0.124

I-234
0.056

I-235
0.035

I-236
0.431

I-237
0.705

I-239
0.035

I-240
0.185

I-241
0.822

I-242
0.357

I-244
0.027

I-245
0.047

I-247
0.015

I-248
0.030

I-249
0.010

I-250
0.029

I-251
0.017

I-252
0.010

I-253
0.193

I-254
0.511

I-255
0.008

I-256
0.023

I-257
0.037

I-258
0.024

I-259
0.030

I-260
0.331

I-261
0.019

I-262
0.016

I-263
0.008

I-264
0.014

I-265
0.028

I-266
0.025

I-267
0.014

I-268
0.032

I-269
0.347

I-271
0.542

I-273
0.491

I-275
0.172

I-276
0.117

I-277
0.342

I-278
0.366

I-279
0.016

I-416
0.322

I-417
0.181

I-418
0.593

I-419
0.032

I-420
0.257

I-421
0.191

I-422
0.361

I-424
0.519

I-425
0.697

I-427
0.331

I-428
0.399

I-429
0.007

I-430
0.153

I-431
0.232

I-433
0.425

I-434
0.125

I-435
0.082

I-436
0.042

I-437
0.111

I-438
0.490

I-439
0.116

I-440
0.035

I-441
0.013

I-442
0.005

I-443
0.006

I-444
0.172

I-445
0.152

I-446
0.338

I-447
0.128

I-448
0.246

I-449
0.013

I-450
0.036

I-451
0.019

I-452
0.026

I-453
0.041

I-454
0.036

I-455
0.014

I-456
0.006

I-457
0.488

I-458
0.699

I-459
0.026

I-460
0.103

I-461
0.036

I-462
0.427

I-463
0.127

I-464
0.453

I-465
0.007

I-466
0.260

I-467
0.286

TABLE 188

Compound
P2X3

No.
IC50 (μM)

I-079
0.023

I-080
0.016

I-081
0.151

I-082
0.650

I-085
0.048

I-089
0.700

I-090
0.555

I-091
0.341

I-092
0.092

I-093
0.756

I-094
0.301

I-095
0.195

I-098
0.370

I-102
0.134

I-103
0.355

I-104
0.424

I-105
0.097

I-108
0.192

I-111
0.624

I-112
0.388

I-113
0.012

I-114
0.012

I-115
0.108

I-116
0.077

I-117
0.383

I-118
0.282

I-119
0.098

I-120
0.074

I-122
0.342

I-123
0.013

I-124
0.011

I-125
0.110

I-126
0.015

I-127
0.049

I-128
0.155

I-129
0.091

I-130
0.476

I-131
0.251

I-132
0.043

I-133
0.367

I-134
0.776

I-135
0.015

I-136
0.015

I-137
0.615

I-138
0.016

I-139
0.930

I-141
0.346

I-142
0.315

I-143
0.331

I-280
0.477

I-281
0.637

I-282
0.472

I-283
0.144

I-284
0.300

I-285
0.648

I-286
0.669

I-288
0.036

I-290
0.051

I-291
0.130

I-292
0.127

I-293
0.012

I-295
0.054

I-296
0.244

I-297
0.220

I-298
0.269

I-299
0.008

I-300
0.114

I-301
0.018

I-302
0.034

I-303
0.031

I-304
0.021

I-305
0.020

I-306
0.054

I-307
0.158

I-308
0.193

I-309
0.182

I-310
0.337

I-311
0.121

I-312
0.054

I-313
0.320

I-314
0.329

I-315
0.252

I-316
0.130

I-317
0.073

I-318
0.328

I-319
0.222

I-320
0.274

I-321
0.070

I-322
0.102

I-323
0.310

I-324
0.109

I-325
0.018

I-326
0.027

I-327
0.093

I-328
0.065

I-329
0.578

I-330
0.070

I-331
0.722

I-468
0.467

I-469
0.646

I-470
0.972

I-471
0.019

I-472
0.007

I-473
0.182

I-474
0.071

I-475
0.181

I-476
0.051

I-477
0.477

I-478
0.034

I-479
0.010

I-480
0.042

I-481
0.378

I-482
0.333

I-483
0.089

I-484
0.091

I-485
0.218

I-486
0.004

I-487
0.167

I-488
0.067

I-489
0.006

I-490
0.017

I-491
0.155

I-492
0.104

I-493
0.105

I-494
0.053

I-495
0.059

I-496
0.055

I-497
0.036

I-498
0.008

I-499
0.398

I-500
0.012

I-501
0.052

I-502
0.067

I-503
0.017

I-504
0.238

I-505
0.168

I-506
0.112

I-507
0.101

I-508
0.133

I-509
0.247

I-510
0.174

I-511
0.117

I-512
0.062

I-513
0.065

I-514
0.138

I-515
0.037

I-516
0.033

TABLE 189

Compound
P2X3

No.
IC50 (μM)

I-144
0.365

I-145
0.016

I-146
0.727

I-147
0.017

I-148
0.073

I-149
0.015

I-150
0.415

I-151
0.008

I-152
0.219

I-153
0.216

I-154
0.192

I-155
0.035

I-156
0.032

I-157
0.025

I-158
0.023

I-159
0.016

I-160
0.013

I-161
0.007

I-162
0.041

I-164
0.074

I-165
0.095

I-166
0.019

I-167
0.013

I-168
0.120

I-169
0.019

I-171
0.610

I-172
0.024

I-173
0.137

I-174
0.572

I-176
0.046

I-178
0.374

I-179
0.659

I-180
0.005

I-181
0.114

I-183
0.004

I-184
0.163

I-185
0.111

I-186
0.013

I-187
0.086

I-188
0.022

I-189
0.014

I-190
0.040

I-191
0.279

I-192
0.612

I-193
0.994

I-194
0.063

I-195
0.235

I-197
0.036

I-198
0.064

I-332
0.281

I-333
0.058

I-334
0.078

I-336
0.351

I-337
0.103

I-338
0.147

I-339
0.892

I-340
0.336

I-341
0.508

I-342
0.067

I-343
0.078

I-344
0.594

I-345
0.999

I-346
0.677

I-347
0.047

I-348
0.055

I-349
0.037

I-350
0.066

I-351
0.101

I-353
0.210

I-354
0.057

I-355
0.044

I-356
0.007

I-357
0.020

I-358
0.025

I-359
0.024

I-360
0.021

I-361
0.048

I-362
0.040

I-363
0.007

I-364
0.009

I-365
0.082

I-366
0.013

I-367
0.019

I-368
0.016

I-369
0.091

I-370
0.194

I-371
0.447

I-372
0.035

I-373
0.051

I-374
0.040

I-375
0.030

I-376
0.025

I-377
0.148

I-378
0.192

I-379
0.118

I-380
0.007

I-381
0.007

I-382
0.006

I-517
0.026

I-518
0.087

I-519
0.033

I-521
0.554

I-523
0.351

I-524
0.696

I-525
0.018

I-526
0.219

I-527
0.039

I-528
0.070

I-530
0.237

I-531
0.286

I-532
0.204

I-533
0.033

I-535
0.049

I-536
0.032

I-537
0.083

I-538
0.119

I-539
0.062

I-540
0.496

I-541
0.010

I-542
0.058

I-543
0.240

I-544
0.008

I-545
0.142

I-546
0.395

I-547
0.217

I-548
0.077

I-549
0.213

I-550
0.254

I-551
0.005

I-552
0.186

I-553
0.337

I-555
0.579

I-556
0.032

I-557
0.444

I-558
0.008

I-559
0.040

I-560
0.275

I-562
0.101

I-563
0.042

I-564
0.018

I-565
0.013

I-566
0.061

I-567
0.057

I-568
0.066

I-569
0.035

I-570
0.070

I-571
0.060

TABLE 190

Compound
P2X3

No.
IC50 (μM)

I-199
0.019

I-200
0.014

I-201
0.039

I-202
0.040

I-204
0.043

I-206
0.630

I-207
0.008

I-208
0.014

I-209
0.234

I-210
0.047

I-211
0.157

I-212
0.092

I-213
0.006

I-214
0.022

I-215
0.013

I-216
0.679

I-217
0.012

I-218
0.073

I-219
0.324

I-220
0.005

I-221
0.081

I-222
0.006

I-223
0.012

I-224
0.073

I-383
0.036

I-384
0.019

I-385
0.227

I-391
0.684

I-392
0.946

I-393
0.015

I-394
0.011

I-395
0.006

I-396
0.007

I-397
0.122

I-398
0.014

I-399
0.044

I-400
0.022

I-401
0.079

I-402
0.080

I-404
0.071

I-405
0.031

I-406
0.029

I-408
0.018

I-409
0.177

I-410
0.151

I-412
0.310

I-413
0.042

I-414
0.268

I-572
0.171

I-573
0.123

I-574
0.280

I-575
0.252

I-576
0.237

I-577
0.047

I-578
0.386

I-579
0.429

I-581
0.466

I-582
0.359

I-583
0.010

I-584
0.167

I-585
0.157

I-586
0.254

I-587
0.374

I-588
0.029

I-589
0.032

I-590
0.028

I-591
0.031

I-592
0.827

I-593
0.811

I-594
0.715

I-597
0.668

I-598
0.785

TABLE 191

Compound
P2X3

No.
IC50 (μM)

II-001
0.104

II-002
0.217

II-003
0.140

II-004
0.378

II-006
0.245

II-007
0.062

II-008
0.505

II-009
0.054

II-010
0.134

II-011
0.319

II-012
0.004

II-013
0.019

II-014
0.017

II-015
0.087

II-016
0.158

II-017
0.054

II-018
0.022

II-019
0.021

II-020
0.008

II-021
0.009

II-022
0.004

II-023
0.004

II-024
0.062

II-025
0.015

II-026
0.023

II-027
0.008

II-028
0.014

II-029
0.090

II-030
0.128

II-031
0.018

II-032
0.006

II-033
0.117

II-034
0.046

II-035
0.006

II-036
0.231

II-037
0.008

II-038
0.014

II-039
0.005

II-040
0.070

II-041
0.027

II-042
0.010

II-043
0.017

II-044
0.582

II-045
0.016

II-046
0.861

II-047
0.011

II-048
0.057

II-049
0.011

II-050
0.007

II-088
0.004

II-089
0.107

II-090
0.002

II-091
0.002

II-092
0.002

II-093
0.002

II-094
0.065

II-095
0.012

II-096
0.223

II-097
0.358

II-098
0.761

II-099
0.046

II-100
0.031

II-101
0.027

II-102
0.076

II-104
0.003

II-105
0.013

II-106
0.226

II-107
0.114

II-108
0.015

II-109
0.021

II-110
0.024

II-111
0.091

II-112
0.389

II-113
0.838

II-114
0.012

II-115
0.011

II-117
0.348

II-118
0.429

II-119
0.137

II-121
0.464

II-123
0.431

II-124
0.008

II-125
0.010

II-126
0.221

II-127
0.004

II-128
0.216

II-130
0.004

II-131
0.088

II-132
0.141

II-133
0.116

II-136
0.055

II-137
0.148

II-138
0.044

II-139
0.332

II-141
0.022

II-142
0.104

II-145
0.033

II-146
0.416

II-189
0.897

II-191
0.322

II-192
0.222

II-193
0.195

II-194
0.392

II-195
0.944

II-196
0.783

II-197
0.106

II-198
0.123

II-199
0.113

II-200
0.448

II-201
0.033

II-202
0.076

II-203
0.028

II-204
0.017

II-205
0.811

II-208
0.112

II-209
0.087

II-210
0.811

II-211
0.135

II-212
0.238

II-213
0.011

II-215
0.015

II-216
0.473

II-217
0.003

II-218
0.005

II-219
0.014

II-220
0.069

II-223
0.023

II-224
0.031

II-225
0.979

II-227
0.034

II-229
0.082

II-231
0.344

II-232
0.016

II-233
0.092

II-234
0.130

II-235
0.017

II-236
0.005

II-237
0.853

II-238
0.019

II-239
0.205

II-240
0.116

II-241
0.213

II-242
0.152

II-243
0.138

II-244
0.144

II-245
0.006

II-246
0.871

TABLE 192

Compound
P2X3

No.
IC50 (μM)

II-051
0.005

II-052
0.033

II-053
0.035

II-054
0.026

II-055
0.548

II-057
0.017

II-058
0.494

II-059
0.046

II-060
0.538

II-061
0.166

II-062
0.112

II-064
0.075

II-067
0.153

II-068
0.508

II-069
0.414

II-072
0.739

II-073
0.105

II-074
0.032

II-075
0.153

II-076
0.012

II-077
0.237

II-078
0.016

II-079
0.011

II-080
0.011

II-081
0.189

II-082
0.044

II-083
0.024

II-084
0.018

II-085
0.023

II-086
0.032

II-087
0.009

II-147
0.977

II-148
0.311

II-149
0.377

II-151
0.650

II-155
0.322

II-156
0.412

II-157
0.524

II-158
0.650

II-159
0.360

II-163
0.034

II-164
0.036

II-165
0.041

II-166
0.007

II-167
0.005

II-168
0.101

II-169
0.004

II-170
0.034

II-171
0.007

II-172
0.011

II-173
0.004

II-174
0.003

II-175
0.003

II-176
0.010

II-178
0.149

II-180
0.262

II-181
0.301

II-182
0.060

II-183
0.460

II-184
0.012

II-185
0.011

II-188
0.156

II-247
0.033

II-248
0.013

II-250
0.043

II-251
0.008

II-253
0.020

II-254
0.002

II-255
0.003

II-256
0.018

II-257
0.033

II-258
0.304

II-259
0.410

II-260
0.036

II-261
0.140

II-262
0.039

II-263
0.108

II-264
0.011

II-265
0.031

II-266
0.007

II-268
0.024

II-269
0.363

II-270
0.025

II-271
0.153

II-272
0.392

II-274
0.019

II-275
0.027

II-277
0.274

II-278
0.013

II-279
0.378

II-280
0.244

II-281
0.664

As shown, the compounds of the invention showed inhibiting activity on P2X₃receptor. Furthermore, as the compounds of the invention are effective to P2X₃subtype, the compounds also have inhibiting activity on P2X₂/₃receptor, which comprises P2X₃subtype.

(CYP3A4 Fluorescent MBI Test)

The CYP3A4 fluorescent MBI test is a test of investigating enhancement of CYP3A4 inhibition of a compound by a metabolism reaction, and the test was performed using, as CYP3A4 enzyme expressed in Escherichia coli and employing, as an index, a reaction in which 7-benzyloxytrifluoromethylchmarin (7-BFC) is debenzylated by the CYP3A4 enzyme to produce a metabolite, 7-hydroxytrifluoromethylchmarin (HFC) emitting fluorescent light.

The reaction conditions were as follows: substrate, 5.6 μmol/L 7-BFC; pre-reaction time, 0 or 30 minutes; reaction time, 15 minutes; reaction temperature, 25° C. (room temperature); CYP3A4 content (expressed in Escherichia cob), at pre-reaction 62.5 μmol/mL, at reaction 6.25 pmol/mL (at 10-fold dilution); test drug concentration, 0.625, 1.25, 2.5, 5, 10, 20 μmol/L (six points).

An enzyme in a K-Pi buffer (pH 7.4) and a test drug solution as a pre-reaction solution were added to a 96-well plate at the composition of the pre-reaction, a part of it was transferred to another 96-well plate so that it was 1/10 diluted by a substrate in a K-Pi buffer, NADPH as a co-factor was added to initiate a reaction as an index (without preincubation) and, after a predetermined time of a reaction, acetonitrile/0.5 mol/L Tris (trishydroxyaminomethane)=4/1 was added to stop the reaction. In addition, NADPH was added to a remaining preincubation solution to initiate a preincubation (with preincubation) and, after a predetermined time of a preincubation, a part was transferred to another plate so that it was 1/10 diluted with a substrate and a K-Pi buffer to initiate a reaction as an index. After a predetermined time of a reaction, acetonitrile/0.5 mol/L Tris (trishydroxyaminomethane)=4/1 was added to stop the reaction. For the plate on which each index reaction had been performed, a fluorescent value of 7-HFC which is a metabolite was measured with a fluorescent plate reader. (Ex=420 nm, Em=535 nm).

Addition of only DMSO which is a solvent dissolving a drug to a reaction system was adopted as a control (100%), remaining activity (%) was calculated at each concentration of a test drug added as the solution, and IC₅₀was calculated by reverse-presumption by a logistic model using a concentration and an inhibition rate. When a difference between IC₅₀values is 5 μM or more, this was defined as (+) and, when the difference is 3 μM or less, this was defined as (−).

(CYP Inhibition Test)

Using commercially available pooled human hepatic microsome, and employing, as markers, 7-ethoxyresorufin O-deethylation (CYP1A2), tolbutamide methyl-hydroxylation (CYP2C9), mephenyloin 4′-hydroxylation (CYP2C19), dextromethorphan O-demethylation (CYP2D6), and terfenedine hydroxylation as typical substrate metabolism reactions of human main five CYP enzyme forms (CYP1A2, 2C9, 2C19, 2D6, 3A4), an inhibitory degree of each metabolite production amount by a test compound was assessed.

The reaction conditions were as follows: substrate, 0.5 μmol/L ethoxyresorufin (CYP1A2), 100 μmol/L tolbutamide (CYP2C9), 50 μmol/L S-mephenitoin (CYP2C19), 5 μmol/L dextromethorphan (CYP2D6), 1 terfenedine (CYP3A4); reaction time, 15 minutes; reaction temperature, 37° C.; enzyme, pooled human hepatic microsome 0.2 mg protein/mL; test drug concentration, 1, 5, 10, 20 μmol/L (four points).

Each five kinds of substrates, human hepatic microsome, or a test drug in 50 mM Hepes buffer as a reaction solution was added to a 96-well plate at the composition as described above, NADPH, as a cofactor was added to initiate metabolism reactions as markers and, after the incubation at 37° C. for 15 minutes, a methanol/acetonitrile=1/1 (v/v) solution was added to stop the reaction. After the centrifugation at 3000 rpm for 15 minutes, resorufin (CYP1A2 metabolite) in the supernatant was quantified by a fluorescent multilabel counter and tributamide hydroxide (CYP2CP metabolite), mephenyloin 4′ hydroxide (CYP2C19 metabolite), dextromethorphan (CYP2D6 metabolite), and terfenadine alcohol (CYP3A4 metabolite) were quantified by LC/MS/MS.

Addition of only DMSO being a solvent dissolving a drug to a reaction system was adopted as a control (100%), remaining activity (%) was calculated at each concentration of a test drug added as the solution and IC₅₀was calculated by reverse presumption by a logistic model using a concentration and an inhibition rate.

(FAT Test)

20 μl of freezing-stored rat typhoid bacillus (Salmonella typhimurium TA98 strain, TA100 strain) was inoculated on 10 mL of a liquid nutrient medium (2.5% Oxoid nutrient broth No. 2), and this was cultured before shaking at 37° C. for 10 hours. 9 mL of a bacterial solution of the TA98 strain was centrifuged (2000×g, 10 minutes) to remove a culturing solution, the bacteria was suspended in 9 mL of a Micro F buffer (K₂HPO₄: 3.5 g/L, KH2PO₄: 1 g/L, (NH₄)₂SO₄: 1 g/L, trisodium citrate dehydrate: 0.25 g/L, MgSO₄.7H₂O: 0.1 g/L), the suspension was added to 110 mL of an Exposure medium (Micro F buffer containing Biotin: 8 μg/mL, histidine: 0.2 μg/mL, glucose: 8 mg/mL), and the TA100 strain was added to 120 mL of the Exposure medium relative to 3.16 mL of the bacterial solution to prepare a test bacterial solution. Each 12 μL of a test substance DMSO solution (8 stage dilution from maximum dose 50 mg/mL at 2-fold ratio), DMSO as a negative control, 50 μg/mL of 4-nitroquinoline-1-oxide DMSO solution for the TA98 strain, 0.25 μg/mL of 2-(furyl)-3-(5-nitro-2-furyl)acrylamide DMSO solution for the TA100 strain under the non-metabolism activating condition, 40 μg/mL of 2-aminoanthracene DMSO solution for the TA98 strain, 20 μg/mL of 2-aminoanthracene DMSO solution for the TA100 strain under the metabolism activating condition as a positive control, and 588 μL of the test bacterial solution (a mixed solution of 498 μl of the test bacterial solution and 90 μL of S9 mix under the metabolism activating condition) were mixed, and this was shaking-cultured at 37° C. for 90 minutes. 460 μL of the bacterial solution exposed to the test substance was mixed with 2300 μL of an Indicator medium (Micro F buffer containing biotin: 8 μg/mL, histidine 0.2 μg/mL, glucose: 8 mg/mL, Bromo Cresol Purple: 37.5 μg/mL), each 50 μL was dispensed into microplate 48 wells/dose, and this was subjected to stationary culturing at 37° C. for 3 days. Since a well containing a bacterium which has obtained the proliferation ability by mutation of an amino acid (histidine) synthesizing enzyme gene turns from purple to yellow due to a pH change, the bacterium proliferation well which has turned to yellow in 48 wells per dose is counted, and was assessed by comparing with a negative control group. (−) means that mutagenicity is negative and (+) is positive.

(Solubility Test)

The solubility of a compound is determined under a condition in which 1% DMSO is added. 10 mM compound solution is prepared using DMSO, and then 6 μL of the compound solution is added to 594 μL of artificial intestinal juice in pH 6.8 (to 250 mL of 0.2 mol/L potassium dihydrogen phosphate reagent solution is added 118 mL of 0.2 mol/L NaOH reagent solution and water to provide a final volume of 1000 mL). After standing at 25 degrees Celsius for 16 hours, the mixed solution is filtrated with suction. The filtrate is diluted twice with methanol/water (1/1), and then a concentration in the filtration is measured with HPLC or LC/MS/MS by the absolute calibration method.

(Metabolism Stability Test)

Using commercially available pooled human hepatic microsomes, a test compound was reacted for a constant time, a remaining rate was calculated by comparing a reacted sample and an unreacted sample, thereby, a degree of metabolism in liver was assessed.

A reaction was performed (oxidative reaction) at 37° C. for 0 minute or 30 minutes in the presence of 1 mmol/L NADPH in 0.2 mL of a buffer (50 mmol/L Tris-HCl pH 7.4, 150 mmol/L potassium chloride, 10 mmol/L magnesium chloride) containing 0.5 mg protein/mL of human liver microsomes. After the reaction, 50 of the reaction solution was added to 100 μl, of a methanol/acetonitrile=1/1 (v/v), mixed and centrifuged at 3000 rpm for 15 minutes. The test compound in the supernatant was quantified by LC/MS/MS, and a remaining amount of the test compound after the reaction was calculated, letting a compound amount at 0 minute reaction time to be 100%. Hydrolysis reaction was performed in the absence of NADPH and glucuronidation reaction was in the presence of 5 mM UDP-glucuronic acid in place of NADPH, followed by similar operations.

(hERG Test)

For the purpose of assessing risk of an electrocardiogram QT interval prolongation, effects on delayed rectifier K+ current (I_Kr), which plays an important role in the ventricular repolarization process, was studied using HEK293 cells expressing human ether-a-go-go related gene (hERG) channel.

After a cell was retained at a membrane potential of −80 mV by whole cell patch clamp method using an automated patch clamp system (PatchXpress 7000A, Axon Instruments Inc.), I_Krinduced by depolarization pulse stimulation at +40 mV for 2 seconds and, further, repolarization pulse stimulation at −50 mV for 2 seconds was recorded. After the generated current was stabilized, extracellular solution (NaCl: 135 mmol/L, KCl: 5.4 mmol/L, NaH₂PO₄: 0.3 mmol/L, CaCl₂.2H₂O: 1.8 mmol/L, MgCl₂.6H₂O: 1 mmol/L, glucose: 10 mmol/L, HEPES (4-(2-hydroxyethyl)-1-piperazineethanesulfonic acid): 10 mmol/L, pH=7.4) in which the test compound had been dissolved at an objective concentration was applied to the cell under the room temperature condition for 10 minutes. From the recording I_Kr, an absolute value of the tail peak current was measured based on the current value at the resting membrane potential using an analysis software (DataXpress ver. 1, Molecular Devices Corporation). Further, the % inhibition relative to the tail peak current before application of the test substance was calculated, and compared with the vehicle-applied group (0.1% dimethyl sulfoxide solution) to assess influence of the test substance on I_Kr.

(Bioavailability (BA) Test)

Materials and Methods for experiment of BA

(1) Animals:

Male Crl: CD(SD) rats of 6 weeks of age are purchased from Charles River Laboratories Japan, Inc., and housed during one week quarantine. Jugular vein c annulation surgery is performed more than 3 days before administration for the rats. The rats are used at 8 weeks of age in the experiments.

(2) Animal Husbandry:

Animal room is maintained under a 12-hr light (8:00-20:00)/dark (20:00-8:00) cycle and kept temperature (20-26° C.) and relative humidity (30-70%). Rats have free access to solid food (CRF-1, Japan Charles River Inc.,) and sterilized bottled tap water.

(3) Identification of Rats and Cage:

Each rat is identified by a tail or a back marked with an oil marker pen and individually housed in a cage labeled with name of the study director, date of receipt, strain, gender and supplier in the experiment. Five rats are housed in one cage before the experiments. One rat is housed in one cage in the experiments.

(4) Setting of Dose and Group Compositions:

Group compositions as shown below, are set by Dose of Oral and Intravenous administration, respectively.

Oral: 1 mg/5 mL/kg (n=2)

Intravenous: 0.5 mg/l mL/kg (n=2)

(5) Preparation for Dosing Formulation:

In oral administration study, a test suspension is prepared by using 0.5% methylcellulose (MC, 400 cP) as test substance. In intravenous administration study, a test solution is prepared by using N,N-dimethylacetoamide (DMA)/propylenglycol (PG)=(1/1) as test substance.

(6) Dosing Procedure:

In oral administration study, the test suspension is dosed to the stomach of rats by using a gavage tube at 5 mL/kg In intravenous administration study, the test solution is dosed to rats via tail vein using a syringe with a needle.

(7) Evaluation Items:

Blood was collected at each time point and separated plasma. Plasma concentration of the test substance is determined by a LC/MS/MS system.

(8) Data Analysis:

Area under the plasma concentration-time curve (AUC) is calculated by means of WinNonline® program, respectively. Bioavailability (BA) is calculated by using AUC values in oral administration study and in intravenous administration study.

Preparation Example 1

A granule containing the following ingredient is prepared.

Ingredient
Compound represented by the formula (I)
10 mg

Lactose
700 mg

Corn starch
274 mg

HPC-L
16 mg

The compound represented by the formula (I) and lactose are passed through a 60 mesh sieve. Corn starch is passed through a 120 mesh sieve. These are mixed with a V-type mixing machine. An aqueous solution of HPC-L (low viscosity hydroxypropylcellulose) is added to a mixture powder, and this is kneaded, granulated (extrusion granulation, pore diameter 0.5 to 1 mm), and dried. The resulting dry granule is sieved with a vibration sieve (12/60 mesh) to obtain a granule.

Preparation Example 2

A powder for filling into a capsule containing the following ingredients is prepared.

Ingredient
Compound represented by the formula (I)
10 mg

Lactose
79 mg

Corn starch
10 mg

Magnesium stearate
1 mg

The compound represented by the formula (I), and lactose are passed through a 60 mesh sieve. Corn starch is passed through a 120 mesh sieve. These and magnesium stearate are mixed with a V-type mixing machine. 10 trituration 100 mg is filled into a No. 5 hard gelatin capsule.

Preparation Example 3

A tablet containing the following ingredients is prepared.

Ingredient
Compound represented by the formula (I)
10 mg

Lactose
90 mg

Microcrystaline cellulose
30 mg

CMC-Na
15 mg

Magnesium stearate
5 mg

The compound represented by the formula (I), lactose, microcrystalline cellulose, CMC-Na (carboxymethylcellulose sodium salt) are passed through a 60 mesh sieve, and mixed. Magnesium stearate is mixed into a mixture powder to obtain a mixture powder for tabletting. The present mixed powder is directly compressed to obtain a 150 mg tablet.

Formulation Example 4

The following ingredients are warmed, mixed, and sterilized to obtain an injectable.

Ingredient
Compound represented by the formula (I)
3
mg

Nonionic surfactant
15
mg

Purified water for injection
1
ml

Formulation Example 5

A cataplasm containing the following ingredients is prepared.

Ingredient
Compound represented by the formula (I)
50 mg

aqueous-based (5% ethanol/5% butylene
950 mg

glycol/90% purified water)

glycerin

kaoline

aqueous polyvinyl alcohol

The compound represented by the formula (I) is added to aqueous-based. The mixture is irradiated by ultrasonic for 15 minutes and then is sufficiently stirred to obtain a solution. 5 part of glycerin, 1 part of kaoline and 5 part of aqueous polyvinyl alcohol are homogeneously mixed and 1 part of the resulting solution is added to the above solution including the compound represented by the formula (I). The obtained solution is mixed and to give a paste form and the resulting paste is applied to an onwoven fabric. The resulting composition is covered by polyester film to give a cataplasm.

INDUSTRIAL APPLICABILITY

The compound of the invention has antagonizing effect on P2X₃and/or P2X₂/₃receptor and is useful in the treatment of diseases or conditions associated with a P2X₃and/or P2X₂/₃receptor, such as chronic pain, overactive bladder, etc.

NOVEL PYROLINONE DERIVATIVE AND PHARMACEUTICAL COMPOSITION COMPRISING THE SAME

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