ORGANIC THIN-FILM EL DEVICE

Abstract

In an organic thin-film EL device of a charge injection type which has an organic thin-film layer contiguous to the surface of the cathode opposite to an anode, said organic thin-film layer is made of an organic compound represented by the following formula (I): 1

Description

BACKGROUND OF THE INVENTION

[0001] 1. Field of the Invention

[0002] This invention relates to an organic thin-film EL device, particularly to a cathode of an organic thin-film EL device having light emitting picture elements arranged in the matrix form.

[0003] 2. Prior Art

[0004] An organic thin-film EL device makes use of the phenomenon that holes injected from an anode and electrons injected from a cathode recombine in an emitter layer and emits light after the excitation state. Although various device structures have been studied according to the properties of the light emitting material of the emitter layer, devices can be fabricated principally by sandwiching between the anode and cathode an organic emitter layer which emits strong fluorescence. For the heightening of luminous efficiency and stable operation, it is considered effective to dispose a charge transport layer such as hole injection transport layer or electron injection transport layer or to carry out doping of guest molecules into an organic emitter layer. Furthermore, electrode materials, particularly, cathode materials are under investigation with a view to improving the luminous efficiency or lifetime properties.

[0005] As a cathode, it is effective to employ an alloy metal having a work function as low as possible. It is reported that from an organic thin-film EL device using, among various alloy metals, lithium-containing aluminum having a low work function, light emission of high efficiency, high luminance and long lifetime is available.

[0006] For example, it is reported in Japanese Patent Application Laid-Open No. 165771/1985 that in an organic thin film having an emitter layer, which is contiguous to a cathode, made of anthracene, light emission with high efficiency is available when an aluminum-lithium alloy or magnesium-lithium alloy is used as a cathode. It is also reported that the optimum content of lithium in the alloy is 1 to 99 wt. %, preferably 10 to 50 wt. %.

[0007] On page 6 of Japanese Patent Application Laid-Open No. 212287/1992, it is reported that light emission with higher luminance can be attained using tris(8-quinolinol) aluminum (which will hereinafter be abbreviated as “Alq”) as an electron transport emitter layer contiguous to a cathode and as the cathode, an alloy containing at least 6 mole % of an alkali metal (for example, an aluminum alloy containing 28 mole % of lithium or magnesium-lithium alloy).

[0008] In Japanese Patent Application Laid-Open No. 121172/1993, it is reported that light emission with high efficiency and long lifetime and EL emission with high environmental stability can be attained in the case where a lithium-aluminum alloy is used as a cathode contiguous to an organic fluorescent thin film made of Alq and this alloy has a lithium concentration of 0.01 to 0.1 wt. %.

[0009] Thus, in an organic thin-film EL device having a cathode made of a lithium-containing alloy, it is considerably important to select a suitable concentration range of lithium to be incorporated in the cathode in accordance with an organic material adjacent to the cathode with a view to imparting the organic thin-film EL device with excellent efficiency and lifetime properties and high environmental resistance.

[0010] An organic thin-film EL device which uses a cathode material containing lithium within a certain composition range exhibits light emission of relatively high luminance and high efficiency.

[0011] In the case where Alq is used as an emitter layer, since Alq emits a green light, light emission on the shorter-wavelength side than it (for example, blue light emission) is not available even by doping into the emitter layer made of Alq. In the case where Alq is used as an electron transport layer, the use of an emitter layer having a large excitation energy or charge injection level (ex. blue-light emitting material) does not permit the sufficient closure of excited electrons or charges, which makes it difficult to attain sufficient luminous efficiency or luminance. The compound of the formula (I) which will be described later is used in this invention in view of such defects.

[0012] The above-described composition range of lithium is used only when an organic thin-film layer adjacent to a cathode is a specific compound (ex. Alq). If an organic thin film made of the compound as represented by the below-described formula (I) is used as an organic thin-film layer adjacent to a cathode, lithium of the above-described composition range does not bring about sufficient luminous efficiency or increases a luminance lowering rate while the resulting element is driven. Such disadvantages occur because the electron injection level of the organic thin film varies depending on the organic material to be employed so that the injection efficiency of electrons is presumed to be insufficient in a known lithium concentration range; and because adhesion between the organic thin film and cathode is weak in the known lithium concentration range, which lowers the electron injection efficiency and makes it difficult to attain stable light emission.

SUMMARY OF THE INVENTION

[0013] An object of the present invention is therefore to provide an organic thin-film EL device which has high efficiency and high luminance, is free from a substantial deterioration in the luminance and has a high yield when producing the same.

[0014] The present inventors have found that an organic thin-film EL device having high luminous efficiency (luminance per current density) and has long lifetime can be obtained using an aluminum alloy containing lithium in a concentration range of 0.05 to 1.5 wt. % as a cathode for the organic thin-film EL device wherein an organic thin film layer adjacent to the cathode contains an organic compound represented by the below-described formula (I).

[0015] In the present invention, there is thus provided an organic thin-film EL device of a charge injection type which has an organic thin film layer adjacent to the surface of a cathode opposite to an anode, said organic thin film layer containing an organic compound represented by the following formula (I): 2

[0016] wherein R1 to R6 each independently represents a hydrogen atom, a halogen atom, an alkyl group, an alkoxy group or a cyano group; L represents a group —OR7 in which R7 representing an alkyl group, a cycloalkyl group, an aromatic group which may contain a nitrogen atom, an aromatic group having a bonding group composed of a metal atom or an oxygen atom, or a ligand of an oxinoid compound having said bonding group; M represents a metal atom; and n stands for an integer of 1 or 2, said cathode comprising aluminum as a main component and lithium in an amount of 0.05 to 1.5 wt. %.

[0017] In another aspect of the present invention, there is also provided an organic thin-film EL device of a charge injection type having an organic thin-film layer adjacent to the surface of a cathode opposite to an anode, said organic thin-film layer containing an organic compound represented by the above-described formula (I) and said cathode comprising magnesium as a main component and lithium in an amount of 0.03 to 1.7 wt. %.

[0018] The present invention makes it possible to heighten the basic properties of the device such as luminous efficiency and lifetime.

[0019] In addition, lithium is contained in the aluminum alloy cathode of the present invention in a concentration range as wide as from 0.05 to 1.5 wt. % so that even a slight difference in the lithium composition does not have a large influence on the properties of the device, which makes it possible to fabricate an organic thin-film EL device in a high yield, more specifically, to widen the area of the device without losing uniform luminance and efficiency. Furthermore, neither corrosion nor black spot appears on the cathode easily.

[0020] On the other hand, lithium is contained in the magnesium alloy cathode of the present invention in a concentration range as wide as from 0.03 to 1.7 wt. % so that similar advantages as described above can be obtained and neither corrosion nor black spot occurs easily on the cathode.

BRIEF DESCRIPTION OF THE DRAWINGS

[0021] FIG. 1 is a schematic cross-sectional view illustrating an organic thin-film EL device of the present invention wherein an organic thin-film layer adjacent to a cathode is an emitter layer;

[0022] FIG. 2 is a schematic cross-sectional view illustrating an organic thin-film EL device of the present invention wherein an organic thin-film layer adjacent to a cathode is an electron injection transport layer;

[0023] FIG. 3 is a schematic cross-sectional view illustrating an organic thin-film EL device of the present invention wherein an organic thin-film layer adjacent to a cathode is an electron injection transport layer containing at least one of the cathode components;

[0024] FIG. 4 is a schematic cross-sectional view of an organic thin-film EL device of the present invention having a cathode protective layer formed on a cathode;

[0025] FIG. 5 is a graph illustrating luminous efficiency and luminance half-life of the cathode of Example 1A as a function of its lithium concentration;

[0026] FIG. 6 is a graph illustrating luminous efficiency and luminance half-life of the cathode of Example 43A as a function of its lithium concentration;

[0027] FIG. 7 is a graph illustrating luminous efficiency and luminance half-life of the cathode of Example 85A as a function of its lithium concentration;

[0028] FIG. 8 is a graph illustrating luminous efficiency and luminance half-life of the cathode of Example 106A as a function of its lithium concentration;

[0029] FIG. 9 is a graph illustrating luminous efficiency and luminance half-life of the cathode of Comparative Example 1A as a function of its lithium concentration;

[0030] FIG. 10 is a graph illustrating luminous efficiency and luminance half-life of the cathode of Comparative Example 2A as a function of its lithium concentration;

[0031] FIG. 11 is a graph illustrating luminous efficiency and luminance half-life of the cathode of Comparative Example 3A as a function of its lithium concentration;

[0032] FIG. 12 is a graph illustrating luminous efficiency and luminance half-life of the cathode of Comparative Example 4A as a function of its lithium concentration;

[0033] FIG. 13 is a graph illustrating luminous efficiency and luminance half-life of the cathode of Example 1B as a function of its lithium concentration;

[0034] FIG. 14 is a graph illustrating luminous efficiency and luminance half-life of the cathode of Example 43B as a function of its lithium concentration;

[0035] FIG. 15 is a graph illustrating luminous efficiency and luminance half-life of the cathode of Example 85B as a function of its lithium concentration;

[0036] FIG. 16 is a graph illustrating luminous efficiency and luminance half-life of the cathode of Example 106B as a function of its lithium concentration;

[0037] FIG. 17 is a graph illustrating luminous efficiency and luminance half-life of the cathode of Comparative Example 1B as a function of its lithium concentration;

[0038] FIG. 18 is a graph illustrating luminous efficiency and luminance half-life of the cathode of Comparative Example 2B as a function of its lithium concentration;

[0039] FIG. 19 is a graph illustrating luminous efficiency and luminance half-life of the cathode of Comparative Example 3B as a function of its lithium concentration; and

[0040] FIG. 20 is a graph illustrating luminous efficiency and luminance half-life of the cathode of Comparative Example 4B as a function of its lithium concentration.

[0041] In each diagram, indicated at numeral 11 is a substrate, 12 an anode, 13 a hole injection layer, 14 a hole transport layer, 15 an emitter layer, 16a an electron injection transport layer of an organic thin-film made of the compound of the formula (I), 16b an electron injection transport layer of an organic thin-film which is made of the compound of the formula (I) and has at least one cathode component doped therein, 17 a cathode and 18 a cathode protective layer.

PREFERRED EMBODIMENTS OF THE INVENTION

[0042] In one embodiment of the present invention, when an organic thin-film layer containing the compound of the formula (I) is brought into contact with a cathode made of an aluminum-lithium alloy, a lithium concentration not less than 0.05 wt. % in the alloy is sufficiently effective for improving luminous efficiency and lifetime properties. At a lithium concentration not less than 0.05 wt. %, neither a marked reduction in luminous efficiency nor noticeably rapid lowering in luminance when operating the same is observed. This owes to the following reasons: while the use of an organic thin film containing the compound of the formula (I) heightens an electron injection level when compared with the use of conventional Alq and is therefore disadvantageous in the injection of electrons at a conventional lithium concentration, the injection of electrons is carried out sufficiently at a lithium concentration not less than 0.05 wt. %; and while the adhesion between the organic thin film containing the compound of the formula (I) and a cathode having the conventional lithium concentration is insufficient, sufficient adhesion can be obtained at a lithium concentration not less than 0.05 wt. %. On the other hand, the upper limit of the lithium concentration is controlled to 1.5 wt. % in the present invention, whereby environmental resistance can be maintained sufficiently. Lithium is considerably corrodible in the air, but the lithium concentration in the aluminum alloy not greater than 1.5 wt. % makes it possible not only to suppress the corrosion-induced lowering in luminous efficiency or lifetime properties but also to suppress the growth of black spots. Accordingly, the lithium concentration suitably ranges from 0.05 to 1.5 wt. %, preferably 0.1 to 0.5 wt. %, more preferably 0.15 to 0.5 wt. %.

[0043] Aluminum to be alloyed with lithium and used as a cathode material may be in the form of a single substance or alloy. As an alloy, a known aluminum alloy can be employed insofar as it does not cause an essential deterioration in the properties of aluminum. In this case, the content of aluminum is preferably 80 wt. % or greater, with 90 wt. % or greater being particularly preferred. Examples of such an aluminum alloy include aluminum-scandium, aluminum-silicon, aluminum-copper, aluminum-magnesium and aluminum-cerium.

[0044] In another aspect of the present invention, when an organic thin-film layer represented by the formula (I) is brought into contact with a cathode made of a magnesium-lithium alloy, sufficient effects can be obtained at the lithium concentration in the alloy not less than 0.03 wt. %. When the lithium concentration is not less than 0.03 wt. %, not only sufficient luminous efficiency can be obtained but also a noticeably rapid lowering in luminance when operating the same is not observed. This is because the adhesion between the organic thin film containing the compound of the formula (I) and the magnesium cathode having a lithium concentration not less than 0.03 wt. % becomes sufficient. When the upper limit of the lithium concentration is set at 1.7 wt. %, sufficient environmental resistance can be maintained. Lithium is considerably corrodible in the air, but the lithium concentration in the magnesium alloy not greater than 1.7 wt. % makes it possible not only to suppress the corrosion-induced lowering in luminous efficiency or lifetime properties but also to suppress the growth of a black spot. Accordingly, the lithium concentration range suitably ranges from 0.03 to 1.7 wt. %, preferably 0.03 to 1.0 wt. %, more preferably 0.4 to 1.0 wt. %.

[0045] Magnesium to be alloyed with lithium and used as a cathode material may be in the form of a single substance or alloy. As an alloy, a known magnesium alloy can be employed insofar as it does not cause an essential deteriorate in the properties of magnesium. In this case, the content of magnesium is preferably 80 wt. % or greater. Examples of such a magnesium alloy include magnesium-aluminum, magnesium-indium and magnesium-silver. The organic thin-film EL device to which the cathode of the present invention is applicable can be imparted with excellent storage stability and physical resistance by disposing a cathode protective layer on the cathode of the present invention.

[0046] When the cathode protective layer is disposed on the cathode of the present invention, the cathode is preferred to have a thickness of 1 to 50 nm. If the cathode has a thickness not less than 1 nm, the organic thin-film layer can be covered completely with the above-described cathode material. The organic thin-film layer can be covered sufficiently with the cathode component when its thickness is 50 nm. An unnecessarily thick cathode is not preferred because it thickens the whole device.

[0047] As the cathode protective layer to be formed on the cathode, an aluminum single substance or aluminum alloy is preferred because it is inexpensive, has excellent corrosion resistance and processability and can provide a low sheet resistance. When an aluminum alloy is used as the cathode protective layer, preferred examples of the substance contained in the alloy include scandium, silicon, manganese and copper from the viewpoints of ease of alloy formation and stability of film formation. Particularly in the fabrication and operation of an organic thin-film EL device or an organic thin-film EL device wherein electrodes are interconnected in the form of matrix (for example, active matrix operation type display), there is room for the improvement of the physical strength in the case of a single aluminum substance. Described specifically, addition of the above-described substance can suppress thermal expansion, thereby improving the physical strength, and particularly when the luminance is large (in other words, when the heat evolution due to light emission is large), not only step breakage but also local unevenness and cracks show a marked decrease. The above-described substance provides apparent advantages when added in an amount of 0.1 to 5 mole % based on an alloy to be formed as the protective layer, because amounts not less than 0.1 mole % have a sufficient influence on various properties such as thermal expansion coefficient, when compared with aluminum alone. Amounts not greater than 5 mole %, on the other hand, prevent occurrence of phase separation between aluminum and the substance. The cathode protective layer is desired to have a thickness of 50 to 3000 nm with a view to preventing the influence of oxygen or moisture on the cathode.

[0048] In the present invention, doping of at least one alloy component contained in the cathode or cathode protective layer into an organic thin film (film containing the compound of the formula (I)) contiguous to the cathode brings about an improvement in the luminous efficiency and at the same time is effective for excellent adhesion and improvement in the operation stability (Japanese Patent Application Laid-Open Nos. 243393/1989 and 274695/1991, Preprints of Lecture on the 44-th Spring Meeting of the Japan Society of Applied Physics and Related Society, 1154, 29p-NK-8(1997).

[0049] In the present invention, the most apparent advantages can be obtained when the organic thin film layer contiguous to the cathode is an emitter layer or an electron injection transport layer.

[0050] The compound represented by the formula (I) is preferred to be contained in an amount not less than 95 mole % in the organic thin film layer contiguous to the cathode. It the amount is not less than 95 mole %, no marked deterioration in properties due to impurities or the like occurs and the object of the present invention can be attained sufficiently.

[0051] When the compound of the formula (I) has an alkyl or alkoxy group as R1 to R2, the number of carbon atoms is preferably 1 to 6, with 1 to 4 being particularly preferred. When R7 represents an alkyl group, the number of carbon atoms is preferably 1 to 6, with 1 to 4 being particularly preferred.

[0052] Examples of the compound represented by the formula (I) include organic metal complexes containing an oxinoid ligand as disclosed in Japanese Patent Application Laid-Open Nos. 214332/1993, 258860/1993, 258862/1993, 198378/1993, 331460/1993, 95620/1997, 13026/1997 and 31455/1997 and European Patent Publication Nos. 765106 and 779765. According to them, these compounds are usable as an emitter layer or electron injection and transport layer.

[0053] Specific examples of the compound of the formula (I) include, but not limited to, those shown in Tables 1 to 18.

TABLE 1
Compound	n	R1	R2	R3	R4	R5	R6	M	L
(1)	2	—CH3	H	H	H	H	H	Al	3
(2)	2	—CH3	H	H	H	H	H	Al	4
(3)	2	—CH3	H	H	H	H	H	Al	5
(4)	2	—CH3	H	H	H	H	H	Al	6
(5)	2	—CH3	H	H	H	H	H	Al	7
(6)	2	—CH3	H	H	H	H	H	Al	8
(7)	2	—CH3	H	H	H	H	H	Al	9
(8)	2	—CH3	H	H	H	H	H	Al	10
(9)	2	—CH3	H	H	H	H	H	Al	11
(10)	2	—CH3	H	H	H	H	H	Al	12
(11)	2	—CH3	H	H	H	H	H	Al	13
(12)	2	—CH3	H	H	H	H	H	Al	14

[0054]

TABLE 2
Compound	n	R1	R2	R3	R4	R5	R6	M	L
(13)	2	—CH3	H	H	H	H	H	Al	15
(14)	2	—CH3	H	H	H	H	H	Al	16
(15)	2	—CH3	H	H	H	H	H	Al	17
(16)	2	—CH3	H	H	H	H	H	Al	18
(17)	2	—CH3	H	H	H	H	H	Al	19
(18)	2	—CH3	H	H	H	H	H	Al	20
(19)	2	—CH3	H	H	H	H	H	Al	21
(20)	2	—CH3	H	H	H	H	H	Al	22
(21)	2	—CH3	H	H	H	H	H	Al	Cl
(22)	2	—C2H5	H	H	H	H	H	Al	23
(23)	2	—C2H5	H	H	H	H	H	Al	24

[0055]

TABLE 3
Compound	n	R1	R2	R3	R4	R5	R6	M	L
(24)	2	—C2H5	H	H	H	H	H	Al	25
(25)	2	—C2H5	H	H	H	H	H	Al	26
(26)	2	—C2H5	H	H	H	H	H	Al	27
(27)	2	—C2H5	H	H	H	H	H	Al	28
(28)	2	—C2H5	H	H	H	H	H	Al	Cl
(29)	2	H	H	H	Cl	H	Cl	Al	29
(30)	2	H	H	H	Cl	H	Cl	Al	30
(31)	2	H	H	H	Cl	H	Cl	Al	31
(32)	2	H	H	H	Cl	H	Cl	Al	32
(33)	2	H	H	H	Cl	H	Cl	Al	33
(34)	2	H	H	H	Cl	H	Cl	Al	34
(35)	2	H	H	H	Cl	H	Cl	Al	35
(36)	2	H	H	H	Cl	H	Cl	Al	36
(37)	2	H	H	H	Cl	H	Cl	Al	37

[0056]

TABLE 4
Compound	n	R1	R2	R3	R4	R5	R6	M	L
(38)	2	H	H	H	CI	H	Cl	Al	38
(39)	2	H	H	H	CI	H	Cl	Al	39
(40)	2	H	H	H	CI	H	Cl	Al	40
(41)	2	H	H	H	Cl	H	Cl	Al	41
(42)	2	H	H	H	CI	H	Cl	Al	42
(43)	2	H	H	H	Cl	H	Cl	Al	43
(44)	2	H	H	H	Cl	H	Cl	Al	44
(45)	2	H	H	H	Cl	H	Cl	Al	45
(46)	2	H	H	H	Cl	H	Cl	Al	46

[0057]

TABLE 5
Compound	n	R1	R2	R3	R4	R5	R6	M	L
(47)	2	H	H	H	Cl	H	Cl	Al	47
(48)	2	CH3	H	H	Cl	H	Cl	Al	48
(49)	2	CH3	H	H	Cl	H	Cl	Al	49
(50)	2	CH3	H	H	Cl	H	Cl	Al	50
(51)	2	CH3	H	H	Cl	H	Cl	Al	51
(52)	2	CH3	H	H	Cl	H	Cl	Al	52
(53)	2	CH3	H	H	Cl	H	Cl	Al	53
(54)	2	CH3	H	H	CN	H	H	Al	54
(55)	2	CH3	H	H	CN	H	H	Al	55
(56)	2	CH3	H	H	Cl	H	Cl	Al	56
(57)	2	CH3	H	H	Cl	H	Cl	Al	57
(58)	2	CH3	H	H	Cl	H	Cl	Al	58
(59)	2	CH3	H	H	Cl	H	Cl	Al	59

[0058]

TABLE 6
Compound	n	R1	R2	R3	R4	R5	R6	M	L
(60)	2	CH3	H	H	Cl	H	Cl	Al	60
(61)	2	CH3	H	H	Cl	H	Cl	Al	61
(62)	2	CH3	H	H	Cl	H	Cl	Al	62
(63)	2	CH3	H	H	Cl	H	Cl	Al	63
(64)	2	CH3	H	H	Cl	H	Cl	Al	64
(65)	2	CH3	H	H	H	CF3	H	Al	65
(66)	2	CH3	H	H	H	H	H	In	66
(67)	2	CH3	H	H	H	H	H	In	67
(68)	2	CH3	H	H	H	H	H	In	68
(69)	2	CH3	H	H	H	H	H	In	69
(70)	2	CH3	H	H	H	H	H	In	70

[0059]

TABLE 7
Compound	n	R1	R2	R3	R4	R5	R6	M	L
(71)	2	CH3	H	H	H	H	H	In	71
(72)	2	CH3	H	H	H	H	H	In	72
(73)	2	CH3	H	H	H	H	H	In	73
(74)	2	CH3	H	H	H	H	H	In	74
(75)	2	CH3	H	H	H	H	H	In	75
(76)	2	CH3	H	H	H	H	H	In	76
(77)	2	CH3	H	H	H	H	H	In	77
(78)	2	CH3	H	H	H	H	H	In	78
(79)	2	CH3	H	H	H	H	H	In	79
(80)	2	CH3	H	H	H	H	H	In	80

[0060]

TABLE 8
Compound	n	R1	R2	R3	R4	R5	R6	M	L
(81)	2	CH3	H	H	H	H	H	In	81
(82)	2	CH3	H	H	H	H	H	In	82
(83)	2	CH3	H	H	H	H	H	In	83
(84)	2	CH3	H	H	H	H	H	In	84
(85)	2	CH3	H	H	H	H	H	In	85
(86)	2	—C2H5	H	H	H	H	H	In	86
(87)	2	—C2H5	H	H	H	H	H	In	87
(88)	2	—C2H5	H	H	H	H	H	In	88
(89)	2	—C2H5	H	H	H	H	H	In	89
(90)	2	—C2H5	H	H	H	H	H	In	90
(91)	2	—C2H5	H	H	H	H	H	In	91
(92)	2	—C2H5	H	H	H	H	H	In	92

[0061]

TABLE 9
Compound	n	R1	R2	R3	R4	R5	R6	M	L
(93)	2	—C2H5	H	H	H	H	H	In	93
(94)	2	—C2H5	H	H	H	H	H	In	94
(95)	2	—C2H5	H	H	H	H	H	In	95
(96)	2	—C2H6	H	H	H	H	H	In	96
(97)	2	—C2h5	H	H	H	H	H	In	97
(98)	2	—C2H5	H	H	H	H	H	In	98
(99)	2	—C2H5	H	H	H	H	H	In	99
(100)	2	—C2H5	H	H	H	H	H	In	100
(101)	2	—C2H5	H	H	H	H	H	In	101

[0062]

TABLE 10
Compound	n	R1	R2	R3	R4	R5	R6	M	L
(102)	2	—C2H5	H	H	H	H	H	In	102
(103)	2	—C2H5	H	H	H	H	H	In	103
(104)	2	—C2H5	H	H	H	H	H	In	104
(105)	2	H	H	H	Cl	H	Cl	In	105
(106)	2	H	H	H	Cl	H	Cl	In	106
(107)	2	H	H	H	Cl	H	Cl	In	107
(108)	2	H	H	H	Cl	H	Cl	In	108
(109)	2	H	H	H	Cl	H	Cl	In	109
(110)	2	H	H	H	Cl	H	Cl	In	110
(111)	2	H	H	H	Cl	H	Cl	In	111
(112)	2	H	H	H	Cl	H	Cl	In	112
(113)	2	H	H	H	Cl	H	Cl	In	113

[0063]

TABLE 11
Com-
pound	n	R1	R2	R3	R4	R5	R6	M	L
(114)	2	H	H	H	Cl	H	Cl	In	114
(115)	2	H	H	H	Cl	H	Cl	In	115
(116)	2	H	H	H	Cl	H	Cl	In	116
(117)	2	H	H	H	Cl	H	Cl	In	117
(118)	2	H	H	H	Cl	H	Cl	In	118
(119)	2	H	H	H	Cl	H	Cl	In	119
(120)	2	H	H	H	Cl	H	Cl	In	120
(121)	2	H	H	H	Cl	H	Cl	In	121
(122)	2	H	H	H	Cl	H	Cl	In	122

[0064]

TABLE 12
Compound	n	R1	R2	R3	R4	R5	R6	M	L
(123)	2	H	H	H	Cl	H	Cl	In	123
(124)	2	CH3	H	H	H	H	H	Ga	124
(125)	2	CH3	H	H	H	H	H	Ga	125
(126)	2	CH3	H	H	H	H	H	Ga	126
(127)	2	CH3	H	H	H	H	H	Ga	127
(130)	2	CH3	H	H	H	H	H	Ga	128
(131)	2	CH3	H	H	H	H	H	Ga	129
(132)	2	CH3	H	H	H	H	H	Ga	130
(133)	2	CH3	H	H	H	H	H	Ga	131
(134)	2	CH3	H	H	H	H	H	Ga	132
(135)	2	CH3	H	H	H	H	H	Ga	133
(136)	2	CH3	H	H	H	H	H	Ga	134

[0065]

TABLE 13
Compound	n	R1	R2	R3	R4	R5	R6	M	L
(137)	2	CH3	H	H	H	H	H	Ga	135
(138)	2	CH3	H	H	H	H	H	Ga	136
(139)	2	CH3	H	H	H	H	H	Ga	137
(140)	2	CH3	H	H	H	H	H	Ga	138
(141)	2	CH3	H	H	H	H	H	Ga	139
(142)	2	CH3	H	H	H	H	H	Ga	140
(143)	2	CH3	H	H	H	H	H	Ga	141
(144)	2	CH3	H	H	H	H	H	Ga	142
(145)	2	CH3	H	H	H	H	H	Ga	143
(146)	2	—C2H5	H	H	H	H	H	Ga	144

[0066]

TABLE 14
Compound	n	R1	R2	R3	R4	R5	R6	M	L
(147)	2	—C2H5	H	H	H	H	H	Ga	145
(148)	2	—C2H5	H	H	H	H	H	Ga	146
(149)	2	—C2H5	H	H	H	H	H	Ga	147
(150)	2	—C2H5	H	H	H	H	H	Ga	148
(151)	2	—C2H5	H	H	H	H	H	Ga	149
(152)	2	—C2H5	H	H	H	H	H	Ga	150
(153)	2	—C2H5	H	H	H	H	H	Ga	151
(154)	2	—C2H5	H	H	H	H	H	Ga	152
(155)	2	—C2H5	H	H	H	H	H	Ga	153
(156)	2	—C2H5	H	H	H	H	H	Ga	154
(157)	2	—C2H5	H	H	H	H	H	Ga	155
(158)	2	—C2H5	H	H	H	H	H	Ga	156

[0067]

TABLE 15
Compound	n	R1	R2	R3	R4	R5	R6	M	L
(159)	2	—C2H5	H	H	H	H	H	Ga	157
(160)	2	—C2H5	H	H	H	H	H	Ga	158
(161)	2	—C2H5	H	H	H	H	H	Ga	159
(162)	2	—C2H5	H	H	H	H	H	Ga	160
(163)	2	—C2H5	H	H	H	H	H	Ga	161
(164)	2	—C2H5	H	H	H	H	H	Ga	162
(165)	2	H	H	H	Cl	H	Cl	Ga	163
(166)	2	H	H	H	Cl	H	Cl	Ga	164
(167)	2	H	H	H	Cl	H	Cl	Ga	165
(168)	2	H	H	H	Cl	H	Cl	Ga	166
(169)	2	H	H	H	Cl	H	Cl	Ga	167
(170)	2	H	H	H	Cl	H	Cl	Ga	168

[0068]

TABLE 16
Com-
pound	n	R1	R2	R3	R4	R5	R6	M	L
(171)	2	H	H	H	Cl	H	Cl	Ga	169
(172)	2	H	H	H	Cl	H	Cl	Ga	170
(173)	2	H	H	H	Cl	H	Cl	Ga	171
(174)	2	H	H	H	Cl	H	Cl	Ga	172
(175)	2	H	H	H	Cl	H	Cl	Ga	173
(176)	2	H	H	H	Cl	H	Cl	Ga	174
(177)	2	H	H	H	Cl	H	Cl	Ga	175
(178)	2	H	H	H	Cl	H	Cl	Ga	176
(179)	2	H	H	H	Cl	H	Cl	Ga	177
(180)	2	H	H	H	Cl	H	Cl	Ga	178

[0069]

TABLE 17
Compound	n	R1	R2	R3	R4	R5	R6	M	L
(181)	2	H	H	H	Cl	H	Cl	Ga	179
(182)	2	H	H	H	Cl	H	Cl	Ga	180
(183)	2	H	H	H	Cl	H	Cl	Ga	181
(184)	2	—CH3	H	H	H	H	H	Al	182
(185)	2	—CH3	H	H	H	H	H	Al	183
(186)	2	CH3	H	H	H	H	H	Ga	184
(187)	2	CH3	H	H	H	H	H	Al	185
(188)	2	—CH3	H	H	H	H	H	Ga	186
(189)	2	H	H	H	H	H	H	Al	187

[0070]

TABLE 18
Compound	n	R1	R2	R3	R4	R5	R6	M	L
(190)	1	H	H	H	H	H	H	Zn	188
(191)	1	H	H	H	H	H	H	Be	189
(192)	1	H	H	H	H	H	H	Be	190
(193)	1	H	H	H	H	H	H	Be	191
(194)	1	H	H	H	H	H	H	Be	192

[0071] Examples of the essential device structure applicable to the organic thin-film EL device having the cathode of the present invention include:

[0072] (1) anode/single or multiple hole injection and transport layer/single or multiple emitter layer/cathode,

[0073] (2) anode/single or multiple emitter layer/single or multiple electron injection transport layer/cathode and (3) anode/single or multiple hole injection and transport layer/single or multiple emitter layer/single or multiple electron injection transport layer/cathode. A protective layer or interface layer may be inserted between the cathode and anode as needed. Or, to the organic thin-film EL device of the present invention, a lens-like structure as described in Japanese Patent Application Laid-Open No. 171892/1997 may be applied with a view to lowering the power consumption and increasing the luminous efficiency.

[0074] The above-described cathode or cathode protective layer may be formed by the resistance-heating system vacuum deposition method or by sputtering a substance to be deposited by using an inert gas ion as shown in Japanese Patent Application Laid-Open No. 19993/1992 with a view to improving the adhesion. In the above-described film formation method of a cathode or cathode protective layer by sputtering, surface migration is large owing to the use of ions having a kinetic energy not less than several eV for the film formation, which makes it possible to form a film having excellent adhesion with an organic thin-film layer. By the selection of appropriate film forming conditions, physical or chemical damages to an organic thin film layer can be reduced and a cathode and cathode protective layer having much more improved adhesion when compared with the conventional ones can be formed. Even if a mixture of metals, the vapor pressure of each of which differs greatly from each other, is used as a target, a difference of the composition between the target and cathode or target and cathode protective layer is not large. Electrodes can be formed uniformly even on a large substrate so that the present invention is of practical utility.

[0075] The present invention will hereinafter be described more specifically, but it should however be born in mind that the present invention is not limited to or by the examples.

EXAMPLE 1A

[0076] FIG. 1 is a schematic cross-sectional view illustrating the structure of an organic thin-film EL device according to a first embodiment of the present invention, wherein an organic thin film contiguous to a cathode 17 is an emitter layer 15. Example 1A of the present invention will next be described with reference to FIG. 1.

[0077] On a glass substrate 11, a film of ITO (indium tin oxide) was formed by the ion plating method. The film was etched into short strips, whereby the glass substrate with an anode 12 was formed. The anode 12 made of ITO had a sheet resistance of 13 Ω/□.

[0078] Organic thin films over the ITO-adhered glass substrate were all formed by the molecular-beam deposition method and the vacuum degree during film formation was set at 2×10−8 Torr or less. At an evaporation rate of 0.05 nm/s, a hole injection layer 13 made of tris(4-(4′-(N,N-di(4-tolyl)amino)styryl) phenyltriphenylamine) (which will hereinafter be abbreviated as “TTPA”) of the following formula: 193

[0079] was formed to a thickness of 35 nm, followed by the formation of a hole transport layer 14 made of N,N′-diphenyl-N,N′-bis(α-naphthyl)-1,1′-biphenyl-4,4′-diamine (which will hereinafter be abbreviated as “α-NPD”) of the following formula: 194

[0080] was formed to a thickness of 25 nm at an evaporation rate of 0.25 nm/s.

[0081] Over the hole transport layer, an emitter layer 15 was formed by the co-deposition method, that is, by evaporating Compound (1) in Table 1 and diphenyl 3,9-perylenedicarboxylate from different deposition sources, respectively. At that time, the evaporation rate was precisely controlled so that the diphenyl 3,9-perylenedicarboxylate was contained in the emitter layer in an amount of 3 mole %, whereby the emitter layer 15 having a thickness of 70 nm was formed.

[0082] Over the emitter layer, a cathode 17 made of an aluminum-lithium alloy was pattern formed at a thickness of 150 nm by the co-deposition method, more specifically, by evaporating aluminum and lithium from different evaporation sources respectively.

[0083] Lastly, the device was sealed in an Ar gas atmosphere. Incidentally, the concentration of lithium in the cathode 17 employed in this example was determined by the inductively coupled plasma emission spectrometry (ICP-AES).

[0084] The organic thin film EL device was electrified and luminous efficiency and lifetime properties (luminance half-life) were evaluated. The luminous efficiency (cd/A) was found from a current density at the time when luminance of 300 cd/m2 was emitted. Lifetime properties were evaluated by causing the light emission of the device by the pulse operation at a pulse frequency of 100 Hz, duty ratio of 50% and peak current density of 10 mA/cm2. While the pulse was off, reverse bias voltage of −10 V was applied.

[0085] FIG. 5 is a graph illustrating the luminous efficiency (&Circlesolid;) and luminance half-life (◯) of the cathode 17 as a function of its lithium concentration. The luminous efficiency varies with the lithium concentration of the cathode 17 and becomes 3.1 to 7.2 cd/A at a concentration range of 0.05 to 1.5 wt. %. Particularly within a concentration range of 0.15 to 0.5 wt. %, the luminous efficiency shows a stable value of about 7 cd/A. The luminance half-life exceeds 500 hours within a concentration range of 0.05 to 1.5 wt. % and above all, it exceeds 1000 hours at a concentration range of 0.1 to 0.5 wt. %. At a concentration range less than 0.05 wt. % or greater than 1.5 wt. %, not only a small luminous efficiency but also a markedly short luminance half-life is observed.

[0086] The adhesion of the cathode 17 was measured by peeling in the crosshatching test. The cathode 17 having a lithium concentration of 0.05 to 1.5 wt. % showed the highest load of 1500 to 1800 gf/24 mm, while that having a lithium concentration less than 0.05 wt. % showed the load of 550 gf/24 mm or less and that having a lithium concentration greater than 1.5 wt. % showed the load of 850 gf/24 mm or less.

[0087] In this example, when the aluminum alloy cathode 17 having a lithium concentration of 0.05 to 1.5 wt. %, good properties were attained and particularly at a lithium concentration of 0.15 to 0.5 wt. %, efficiency was high and lifetime properties were stable. This result suggests that an organic thin-film EL device having excellent properties can be obtained by incorporating Compound (1) in the thin-film emitter layer 15 contiguous to the aluminum-lithium cathode 17 and setting the lithium concentration in the cathode 17 at a range of 0.05 to 1.5 wt. %, preferably 0.10 to 0.5 wt. %, more preferably 0.15 to 0.5 wt. %.

EXAMPLES 2A TO 42A

[0088] In each of Examples 2A to 42A, except that the emitter layer 15 having a thickness of 70 nm was formed by a co-deposition method in which each of the compounds shown in Table 19 and 20 instead of Compound (1), as the compound of the formula (I) and diphenyl 3, 9-perylenedicarboxylate were evaporated from different deposition sources, respectively, wherein the evaporation rate was precisely controlled so that the diphenyl 3, 9-perylenedicarboxylate was contained in the emitter layer 15 in an amount of 3 mole %, an organic thin-film EL device was formed in a similar manner to Example 1A, and its properties were evaluated. Results are shown in Tables 19 and 20.

[0089] Even if any one of the above-described compounds were used for the emitter layer 15, when the aluminum-lithium alloy cathode 17 had a lithium concentration ranging from 0.05 to 1.5 wt. %, luminous efficiency became about twice and luminance half-life became about three to five times when compared with those at a lithium concentration less than 0.05 wt. % or greater than 1.5 wt. %. The lithium concentration which is regarded as most suited in Comparative Example 1A is as small as 0.01 to 0.1 wt. % and its range is very narrow, while in this example, the most suited lithium concentration is as wide as 0.05 to 1.5 wt. % and good light-emitting properties are attained. This suggests that when the compound represented by the formula (I) is used for the emitter layer 15 contiguous to the cathode 17, excellent advantages can be obtained at a lithium concentration adjusted to 0.05 to 1.5 wt. %.

[0090] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. The cathode 17 having a lithium concentration of 0.05 to 1.5 wt. % showed the highest load of 1200 to 1800 gf/24 mm, while that having a lithium concentration less than 0.05 wt. % showed the load of 550 gf/24 mm or less and that having a lithium concentration greater than 1.5 wt. % showed the load of 850 gf/24 mm or less.

[0091] The above results indicate that when the compound of the formula (I) is used for the emitter layer 15 contiguous to the cathode 17, improved adhesion, high efficiency and long-life light emission can be attained by adjusting the lithium concentration in the aluminum-lithium alloy cathode 17 at 0.05 to 1.5 wt. %.

COMPARATIVE EXAMPLE 1A

[0092] Except that the emitter layer 15 having a thickness of 70 nm was formed by a co-deposition method in which conventionally and ordinarily used Alq and diphenyl 3, 9-perylenedicarboxylate were evaporated from different deposition sources, respectively, wherein the evaporation rate was precisely controlled so that the diphenyl 3, 9-perylenedicarboxylate was contained in the emitter layer 15 in an amount of 3 mole %, an organic thin-film EL device was formed in a similar manner to Example 1A, and its properties were evaluated.

[0093] As a result, it was observed, as illustrated in FIG. 9, that luminous efficiency and lifetime properties each showed a peak between the lithium concentration of 0.01 and 0.1 wt. %. At the lithium concentration exceeding 0.1 wt. %, a drastic deterioration in light-emitting properties was observed.

[0094] When the adhesion of the cathode portion was measured by peeling in the crosshatching test. As a result, the load was 1000 to 1200 gf/24 mm and showed the highest value when the cathode 17 having a lithium concentration of 0.01 to 0.1 wt. % was employed, while it was 900 gf/24 mm or less when the cathode 17 having a lithium concentration exceeding 0.1 wt. % was employed.

Example 43A

[0095] FIG. 2 is a schematic cross-sectional view illustrating the structure of an organic thin-film EL device according to the second embodiment of the present invention, wherein an organic thin film contiguous to a cathode 17 is an electron injection transport layer 16a and the functions of an emitter layer 15 and electron transport layer 16a are essentially separated.

[0096] Example 43A of the present invention will next be described with reference to FIG. 2. On a glass substrate 11, an ITO (indium tin oxide) film was formed by the ion plating method, followed by etching into short strips, whereby a glass substrate with an anode 12 was formed. The anode 12 made of ITO had a sheet resistance of 13 Ω/□. Organic thin films over the ITO-applied glass substrate were all formed by the molecular-beam deposition method and the vacuum degree during the film formation was set at 2×10−8 Torr or less.

[0097] A hole injection layer 13 made of TTPA was then formed to a thickness of 35 nm at an evaporation rate of 0.05 nm/s, followed by the formation of a hole transport layer 14 made of α-NPD to a thickness of 15 nm at an evaporation rate of 0.25 nm/s.

[0098] Over the hole transport layer, an emitter layer 15 made of 9,10-bis(4-(4-(N,N-di(4-tolyl)aminophenyl)benzyliden)anthracene (which will hereinafter be abbreviated as “BPBA”) represented by the following formula: 195

[0099] was formed to a thickness of 48 nm at an evaporation rate of 0.07 nm/s.

[0100] Over the emitter layer 15, an electron injection transport layer 16a made of the compound (1) in Table 1 was formed to a thickness of 35 nm at an evaporation rate of 0.2 nm/s.

[0101] Then, a cathode 17 made of an aluminum-lithium alloy was pattern-formed to a thickness of 150 nm over the electron injection transport layer by the co-deposition method in which aluminum and lithium were evaporated from different evaporation sources respectively.

[0102] Finally, the resulting device was sealed in an Ar gas atmosphere. In Example 43A, the concentration of lithium in the cathode 17 was determined by ICP-AES.

[0103] The organic thin-film EL device so formed was electrified and luminous efficiency and lifetime properties (luminance half-life) were evaluated. The luminous efficiency (cd/A) was found from a current density at the time when luminance of 300 cd/m2 was emitted. Lifetime properties were evaluated by causing the light emission of the device by the pulse operation at a pulse frequency of 100 Hz, duty ratio of 50% and peak current density of 10 mA/cm2. While the pulse was off, reverse bias voltage of −10 V was applied.

[0104] FIG. 6 is a graph illustrating the luminous efficiency (&Circlesolid;) and luminance half-life (◯) of the cathode 17 as a function of its lithium concentration. The luminous efficiency varies with the lithium concentration of the cathode 17 and becomes 4.3 to 8.5 cd/A at a concentration range of 0.05 to 1.5 wt. %. Particularly within a concentration range of 0.1 to 0.5 wt. %, the luminous efficiency is as high as 8 cd/A or greater. The luminance half-life exceeds 500 hours within a concentration range of 0.05 to 1.5 wt. % and above all, it exceeds 1000 hours at a concentration range of 0.1 to 0.5 wt. %. At a concentration outside the above range, that is, a range less than 0.05 wt. % or greater than 1.5 wt. %, not only a small luminous efficiency but also a markedly short luminance half-life as short as 100 hours or less are observed. Such a lithium concentration outside the above range cannot be employed practically.

[0105] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. The cathode 17 having a lithium concentration ranging from 0.05 to 1.5 wt. % showed the highest load of 1500 to 1800 gf/24 mm, while that having a lithium concentration less than 0.05 wt. % showed the load of 550 gf/24 mm or less and that having a lithium concentration greater than 1.5 wt. % showed the load of 850 gf/24 mm or less.

[0106] In this Example 43A, when the aluminum alloy cathode 17 having a lithium concentration of 0.05 to 1.5 wt. %, good properties were attained and particularly at a lithium concentration of 0.1 to 0.5 wt. %, efficiency was high and lifetime properties were stable. This result suggests that, with respect to organic thin-film EL devices having the device structure shown in FIG. 2, an organic thin-film EL device having excellent properties can be obtained by incorporating Compound (1) of Table 1 in the electron injection transport layer 16a contiguous to the cathode 17 made of an aluminum-lithium alloy and setting the lithium concentration in the cathode 17 at a range of 0.05 to 1.5 wt. %, preferably 0.1 to 0.5 wt. %.

EXAMPLES 44A TO 84A

[0107] In each of Examples 44A to 84A, in a similar manner to Example 43A except that each of the compounds shown in Tables 21 and 22 was used as the compound of the formula (I) for forming the electron injection transport layer 16a of FIG. 2, an organic thin-film EL device was formed and its properties were evaluated. Results are shown in Tables 21 and 22.

[0108] Even if any one of the above-described compounds were employed as the hole injection transport layer 16a, when the aluminum-lithium alloy cathode 17 had a lithium concentration ranging from 0.05 to 1.5 wt. %, luminous efficiency became about twice and luminance half-life became about three to five times when compared with those at a lithium concentration less than 0.05 wt. % or greater than 1.5 wt. %. The lithium concentration which is regarded as most suited in Comparative Example 2A is as small as 0.01 to 0.1 wt. % and its range is very narrow, while in this example, the most suited lithium concentration is as wide as 0.05 to 1.5 wt. % and good light-emitting properties are attained. This suggests that when the compound represented by the formula (I) is used for an electron injection transport layer 16a contiguous to the cathode 17, excellent advantages can be obtained at a lithium concentration adjusted to 0.05 to 1.5 wt. %.

[0109] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. The cathode 17 having a lithium concentration of 0.05 to 1.5 wt. % showed the highest load of 1200 to 1800 gf/24 mm, while that having a lithium concentration less than 0.05 wt. % showed the load of 550 gf/24 mm or less and that having a lithium concentration greater than 1.5 wt. % showed the load of 850 gf/24 mm or less.

[0110] The above results suggest that when the compound of the formula (I) is used for the electron injection transport layer 16a contiguous to the cathode 17, improved adhesion, high efficiency and long-life light emission can be attained by adjusting the lithium concentration in the cathode 17 made of an aluminum-lithium alloy at 0.05 to 1.5 wt. %.

COMPARATIVE EXAMPLE 2A

[0111] In a similar manner to Example 43A except that conventionally and ordinarily used Alq was used for forming an electron injection transport layer 16a, an organic thin-film EL device was formed and its properties were evaluated. As a result, it was observed, as illustrated in FIG. 10, that luminous efficiency and lifetime properties each showed a peak between the lithium concentration of 0.01 and 0.1 wt. %. At the lithium concentration exceeding 0.1 wt. %, a drastic deterioration in light emitting properties was observed.

[0112] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. As a result, the load was 1000 to 1200 gf/24 mm and showed the highest value when the cathode 17 having a lithium concentration of 0.01 to 0.1 wt. % was employed, while it was 900 gf/24 mm when the cathode 17 having a lithium concentration exceeding 0.1 wt. % was employed.

EXAMPLE 85A

[0113] FIG. 3 is a schematic cross-sectional view illustrating the structure of an organic thin-film EL device according to a third embodiment of the present invention, which is different from the structure of the second embodiment in that at least one of the cathode components is contained in the electron injection transport layer 16b contiguous to the cathode 17.

[0114] Example 85A of the present invention will next be described with reference to FIG. 3. On a glass substrate 11, an ITO (indium tin oxide) film was formed by the ion plating method, followed by etching into short strips, whereby a glass substrate with an anode 12 was formed. The anode 12 made of ITO had a sheet resistance of 13 Ω/□. Organic thin films over the ITO-applied glass substrate were all formed by the molecular-beam deposition method and the vacuum degree during film formation was set at 2×10−8 Torr or less.

[0115] A hole injection layer 13 made of TTPA was then formed to a thickness of 35 nm at an evaporation rate of 0.05 nm/s, followed by the formation of a hole transport layer 14 made of α-NPD to a thickness of 25 nm at an evaporation rate of 0.25 nm/s.

[0116] Over the hole transport layer, an emitter layer 15 made of BPBA was formed to a thickness of 48 nm at an evaporation rate of 0.07 nm/s. Over the emitter layer 15, an electron injection transport layer 16b containing 1.5 wt. % of lithium was formed to a thickness of 35 nm by the co-deposition method in which lithium and the compound (1) were evaporated as electron transport materials from different evaporation sources, respectively.

[0117] Then, a cathode 17 made of an aluminum-lithium alloy was pattern-formed to a thickness of 150 nm over the electron injection transport layer by the co-deposition method in which aluminum and lithium were evaporated from different evaporation sources respectively.

[0118] Finally, the resulting element was sealed in an Ar gas atmosphere. In Example 85A, the concentration of lithium in the cathode 17 was studied and determined by ICP-AES.

[0119] FIG. 7 is a graph illustrating the luminous efficiency (&Circlesolid;) and luminance half-life (◯) of the cathode 17 as a function of its lithium concentration. The luminous efficiency varies with the lithium concentration of the cathode 17 and becomes 5 to 9.5 cd/A at a concentration range of 0.05 to 1.5 wt. %. Particularly within a concentration range of 0.1 to 0.5 wt. %, the luminous efficiency is as high as 9 cd/A or greater. The luminance half-life exceeds 600 hours within a concentration range of 0.05 to 1.5 wt. % and above all, it exceeds 1000 hours at a concentration range of 0.1 to 0.5 wt. %. At a concentration outside the above range, that is, a range less than 0.05 wt. % or greater than 1.5 wt. %, on the other hand, not only luminous efficiency but also luminance half-life decreases to half or less of that within the above-described concentration range and luminance half-life becomes even 300 hours or less. In addition, in this Example 85A, the luminous efficiency and lifetime properties shows about a 10% improvement when compared with those of Example 43A. Such an improvement in the properties was brought about by doping lithium, which is one of the cathode components, into the electron injection transport layer 16b of the organic thin-film EL device of the present invention.

[0120] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. The cathode 17 having a lithium concentration of 0.05 to 1.5 wt. % showed the highest load of 1800 to 2200 gf/24 mm, while that having a lithium concentration less than 0.05 wt. % showed the load of 1000 gf/24 mm and that having a lithium concentration greater than 1.5 wt. % showed the load of 1200 gf/24 mm. When compared with Example 43A, the adhesion was improved by about 1.3 times. Such an improvement in the properties was brought about by doping 4 lithium, which is one of the cathode components, into the electron injection transport layer 16b of the present invention, thereby improving the adhesion.

[0121] In this Example, when the aluminum cathode 17 had a lithium concentration of 0.05 to 1.5 wt. %, properties were good and particularly at a lithium concentration of 0.1 to 0.5 wt. %, luminous efficiency was high and lifetime properties were stable. This result suggests that, with respect to organic thin-film EL devices having the device structure shown in FIG. 3, an organic thin-film EL device having-excellent properties can be obtained by incorporating the compound (1) in the electron injection transport layer 16b contiguous to the cathode 17 made of an aluminum and lithium alloy and setting the lithium concentration in the cathode 17 at a range of 0.05 to 1.5 wt. %, preferably 0.1 to 0.5 wt. %.

EXAMPLES 86A TO 105A

[0122] In each of Examples 86A to 105A, in a similar manner to Example 85A except that each of the compounds shown in Tables 23 was used for the electron injection transport layer 16b of FIG. 3, an organic thin-film EL device was formed and its properties were evaluated. The results are shown in Tables 23.

[0123] Even if any one of the above-described compounds were used for the electron injection transport layer 16b, when the aluminum-lithium alloy cathode 17 had a lithium concentration ranging from 0.05 to 1.5 wt. %, luminous efficiency became about twice and luminance half-life became about three to five times when compared with those at a lithium concentration less than 0.05 wt. % or greater than 1.5 wt. %. The lithium concentration which is regarded as most suited in Comparative Example 3A is as small as 0.01 to 0.1 wt. % and its range is very narrow, while in this example, the most suited lithium concentration is as wide as 0.05 to 1.5 wt. % and good light-emitting properties are attained. This suggests that when the compound represented by the formula (I) is used for the electron injection transport layer 16b contiguous to the cathode, excellent advantages can be obtained at a lithium concentration adjusted to 0.05 to 1.5 wt. %.

[0124] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. The cathode 17 having a lithium concentration of 0.05 to 1.5 wt. % showed the highest load of 1800 to 2200 gf/24 mm, while that having a lithium concentration less than 0.05 wt. % showed the load of 550 gf/24 mm or less and that having a lithium concentration greater than 1.5 wt. % showed the load of 850 gf/24 mm or less.

[0125] The above results suggest that when the compound of the formula (I) is used for the electron injection transport layer 16b contiguous to the cathode 17, improved adhesion, high efficiency and long-life light emission can be attained by adjusting the lithium concentration in the cathode 17 made of an aluminum-lithium alloy at 0.05 to 1.5 wt. %.

COMPARATIVE EXAMPLE 3A

[0126] In a similar manner to Example 85A except that the electron injection transport layer 16b was formed by doping lithium into a layer composed of conventionally and ordinarily used Alq, an organic thin-film EL device was formed and its properties were evaluated. As a result, it was observed, as illustrated in FIG. 11, that luminous efficiency and lifetime properties each showed a peak within the lithium concentration ranging from 0.01 to 0.1 wt. %. At the lithium concentration exceeding 0.1 wt. %, a drastic deterioration in light emitting properties was observed.

[0127] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. As a result, the load was 1000 to 1200 gf/24 mm and showed the highest value when the cathode 17 having a lithium concentration of 0.01 to 0.1 wt. % was employed, while it was 900 gf/24 mm or less when the cathode 17 having a lithium concentration exceeding 0.1 wt. % was employed.

EXAMPLE 106A

[0128] FIG. 4 is a schematic cross-sectional view illustrating the structure of an organic thin-film EL device according to a fourth embodiment of the present invention, which is different from the structures of the other embodiments in that a cathode protective layer 18 is disposed over a cathode 17.

[0129] Example 106A of the present invention will next be described with reference to FIG. 4. On a glass substrate 11, an ITO (indium tin oxide) film was formed by the ion plating method, followed by etching into short strips, whereby a glass substrate with an anode 12 was formed. The anode 12 made of ITO had a sheet resistance of 13 Ω/□. Organic thin films over the ITO-applied glass substrate were all formed by the molecular-beam deposition method and the vacuum degree during the film formation was set at 2×10−8 Torr or less.

[0130] A hole injection layer 13 made of TTPA was then formed to a thickness of 35 nm at an evaporation rate of 0.05 nm/s, followed by the formation of a hole transport layer 14 made of α-NPD to a thickness of 15 nm at an evaporation rate of 0.25 nm/s.

[0131] Over the hole transport layer, an emitter layer 15 made of BPBA was formed to a thickness of 48 nm at an evaporation rate of 0.07 nm/s. Over the emitter layer 15, an electron injection transport layer 16a composed of the compound (1) was formed to a thickness of 35 nm at an evaporation rate of 0.2 nm/s.

[0132] Over the electron injection transport layer, a cathode 17 made of an aluminum-scandium-lithium alloy was pattern-formed to a thickness of 30 nm by the co-deposition method in which aluminum containing 1.5 wt. % of scandium and lithium were evaporated from different evaporation sources respectively.

[0133] Over the cathode, an aluminum-scandium alloy containing 1.5 wt. % of scandium was formed to a thickness of 300 nm as a protective layer 18 for the cathode 17 by the RF sputtering in an argon gas.

[0134] Finally, the resulting device was sealed in an Ar gas atmosphere. In Example 106A, the concentrations of lithium and scandium in the cathode 17 were determined by ICP-AES.

[0135] FIG. 8 is a graph illustrating the luminous efficiency (&Circlesolid;) and luminance half-life (◯) of the cathode 17 as a function of its lithium concentration. The luminous efficiency varies with the lithium concentration of the cathode 17 and becomes 6 to 10.5 cd/A at a concentration range of 0.05 to 1.5 wt. %. Particularly within a concentration range as wide as 0.1 to 0.5 wt. %, the luminous efficiency is as high as about 10 cd/A. The luminance half-life exceeds 800 hours within a concentration range of 0.05 to 1.5 wt. % and above all, it exceeds 1500 hours at a concentration range of 0.1 to 0.5 wt. %. At a concentration outside the above range, that is, at a concentration less than 0.05 wt. % or greater than 1.5 wt. %, not only the luminous efficiency but also luminance half-life decreases to half of that within the above-described range and luminance half-life becomes even to 300 hours or less.

[0136] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. The cathode 17 having a lithium concentration of 0.05 to 1.5 wt. % showed the highest load of 1800 to 2200 gf/24 mm, while that having a lithium concentration less than 0.05 wt. % showed the load of 1000 gf/24 mm and that having a lithium concentration greater than 1.5 wt. % showed the load of 1200 gf/24 mm.

[0137] In this Example, when the cathode 17 made of a scandium-containing aluminum-lithium alloy had a lithium concentration of 0.05 to 1.5 wt. %, good properties were attained and particularly at a lithium concentration of 0.1 to 0.5 wt. %, luminous efficiency was high and lifetime properties were stable. This result suggests that, with respect to organic thin-film EL devices having the device structure shown in FIG. 4, an organic thin-film EL device having excellent properties can be obtained by incorporating the Compound (1) in the electron injection transport layer 16a contiguous to the cathode 17 made of a scandium-containing aluminum-lithium alloy and setting the lithium concentration in the cathode 17 at a range of 0.05 to 1.5 wt. %, preferably 0.1 to 0.5 wt. %.

EXAMPLES 107A TO 126A

[0138] In each of Examples 107A to 126A, in a similar manner to Example 106A except that each of the compounds shown in Tables 24 was used for the electron injection transport layer 16a of FIG. 4, an organic thin-film EL device was formed and its properties were evaluated. The results are shown in Tables 24.

[0139] Even if any one of the above-described compounds was employed for the electron injection transport layer 16a, when the cathode 17 made of a scandium-containing aluminum-lithium alloy had a lithium concentration ranging from 0.05 to 1.5 wt. %, luminous efficiency became about twice and luminance half-life became about three to five times when compared with those at a lithium concentration less than 0.05 wt. % or greater than 1.5 wt. %. The lithium concentration which is regarded as most suited in Comparative Example 4A is as small as 0.01 to 0.1 wt. % and its range is very narrow, while in this example, the most suited lithium concentration is as wide as 0.05 to 1.5 wt. % and good light-emitting properties are attained. This suggests that when the compound represented by the formula (I) is used for the electron injection transport layer 16a contiguous to the cathode 17, excellent advantages can be obtained at a lithium concentration adjusted to 0.05 to 1.5 wt. %.

[0140] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. The cathode 17 having a lithium concentration of 0.05 to 1.5 wt. % showed the highest load of 1800 to 2200 gf/24 mm, while that having a lithium concentration less than 0.05 wt. % showed the load of 550 gf/24 mm or less and that having a lithium concentration greater than 1.5 wt. % showed the load of 850 gf/24 mm or less.

[0141] The above results suggest that when the compound of the formula (I) is used for the electron injection transport layer 16a contiguous to the cathode 17, improved adhesion can be attained by setting the lithium concentration in the scandium-containing aluminum-scandium-lithium alloy cathode 17 at 0.05 to 1.5 wt. % and high efficiency and emission of long lifetime can be attained by disposing the cathode protective layer 18 on the cathode 17.

COMPARATIVE EXAMPLE 4A

[0142] In a similar manner to Example 106A except that the electron injection transport layer 16a was made of the conventionally and ordinarily used Alq, an organic thin-film EL device was formed and its properties were evaluated.

[0143] As a result, it was observed, as illustrated in FIG. 12, that luminous efficiency and lifetime properties each showed a peak within a lithium concentration range from 0.01 to 0.1 wt. %. At the lithium concentration exceeding 0.1 wt. %, a drastic deterioration in luminous properties was observed.

[0144] The adhesion of the cathode portion was measured by peeling in the crosshatching test. As a result, the load was 1000 to 1200 gf/24 mm and showed the highest value when the cathode 17 having a lithium concentration of 0.01 to 0.1 wt. % was employed, while it was 900 gf/24 mm when the cathode 17 having a lithium concentration exceeding 0.1 wt. % was employed.

	TABLE 19
	Luminous Efficiency (Maximum Value)	Luminance Half-life (Maximum Value)
	Relative to Li Concentration (cd/A)	Relative to Li Concentration (h)
	Compound	Less than		More than	Less than		More than
	No.	0.05 wt %	0.05˜1.5 wt %	1.5 wt %	0.05 wt %	0.05˜1.5 wt %	1.5 wt %
Example1A	(1)	<3.9	7.2	<3.1	<500	1350	<380
Example2A	(4)	<4.0	7.8	<3.5	<360	1500	<450
Example3A	(5)	<3.5	6.5	<3.0	<360	1400	<400
Example4A	(15)	<2.5	5.5	<3.0	<240	1000	<400
Example5A	(17)	<2.5	5.0	<2.5	<120	950	<240
Example6A	(18)	<3.0	5.5	<3.0	<200	1000	<240
Example7A	(19)	<3.5	6.0	<3.0	<300	1150	<350
Example8A	(22)	<3.8	6.8	<3.0	<300	1100	<400
Example9A	(25)	<4.0	7.5	<3.0	<450	1500	<400
Example10A	(26)	<4.0	7.0	<3.0	<400	1200	<360
Example11A	(29)	<3.0	5.5	<3.5	<250	800	<280
Example12A	(32)	<3.5	6.0	<3.5	<350	950	<350
Example13A	(48)	<3.5	6.5	<3.0	<280	800	<300
Example14A	(62)	<3.5	6.0	<3.5	<300	750	<250
Example15A	(63)	<3.5	6.0	<3.0	<350	700	<300
Example16A	(66)	<2.8	5.5	<2.5	<250	680	<280
Example17A	(69)	<3.0	6.0	<3.0	<380	780	<400
Example18A	(70)	<3.0	6.5	<3.5	<400	680	<300
Example19A	(72)	<2.5	5.8	<2.8	<300	600	<280
Example20A	(80)	<2.4	5.0	<2.5	<250	550	<180
Example21A	(82)	<2.2	4.5	<1.8	<150	350	<150

[0145]

	TABLE 20
	Luminous Efficiency (Maximum Value)	Luminance Half-life (Maximum Value)
	Relative to Li Concentration (cd/A)	Relative to Li Concentration (h)
	Compound	Less than		More than	Less than		More than
	No.	0.05 wt %	0.05˜1.5 wt %	1.5 wt %	0.05 wt %	0.05˜1.5 wt %	1.5 wt %
Example22A	(83)	<2.4	5.0	<2.5	<100	450	<100
Example23A	(84)	<2.4	5.0	<3.0	<80	500	<150
Example24A	(86)	<2.5	4.8	<3.0	<260	600	<150
Example25A	(87)	<2.0	4.2	<1.8	<48	280	<48
Example26A	(93)	<1.8	3.6	<1.5	<48	300	<48
Example27A	(96)	<1.5	3.2	<1.5	<48	350	<72
Example28A	(107)	<1.5	3.5	<1.2	<72	400	<48
Example29A	(119)	<1.8	3.2	<1.5	<96	300	<72
Example30A	(121)	<1.5	3.0	<1.5	<48	280	<24
Example31A	(122)	<3.0	5.0	<2.5	<80	480	<120
Example32A	(124)	<3.5	6.0	<3.0	<180	880	<240
Example33A	(127)	<3.5	6.8	<3.5	<240	960	<300
Example34A	(130)	<3.5	6.0	<3.0	<240	960	<240
Example35A	(133)	<2.8	5.2	<3.0	<120	750	<180
Example36A	(140)	<2.4	4.5	<2.8	<120	600	<240
Example37A	(142)	<2.4	4.0	<2.6	<120	500	<96
Example38A	(143)	<3.0	5.0	<2.8	<300	650	<280
Example39A	(144)	<2.6	4.6	<3.4	<280	580	<120
Example40A	(146)	<3.2	5.5	<3.5	<280	720	<240
Example41A	(165)	<3.0	5.0	<3.5	<240	680	<240
Example42A	(169)	<3.0	5.6	<3.4	<300	720	<240

[0146]

	TABLE 21
	Luminous Efficiency (Maximum Value)	Luminance Half-life (Maximum Value)
	Relative to Li Concentration (cd/A)	Relative to Li Concentration (h)
	Compound	Less than		More then	Less than		More than
	No.	0.05 wt %	0.05˜1.5 wt %	1.5 wt %	0.05 wt %	0.05˜1.5 wt %	1.5 wt %
Example43A	(1)	<4.2	8.5	<4.3	<450	1380	<185
Example44A	(4)	<4.5	9.0	<4.5	<460	1200	<240
Example45A	(5)	<4.0	7.8	<4.0	<300	1100	<200
Example46A	(18)	<3.5	6.5	<3.8	<240	1000	<240
Example47A	(19)	<4.0	7.2	<3.5	<320	1150	<240
Example48A	(21)	<3.5	5.8	<3.2	<180	850	<120
Example49A	(22)	<4.0	6.5	<3.5	<240	950	<240
Example50A	(25)	<4.5	7.5	<4.0	<300	1200	<300
Example51A	(26)	<4.2	7.0	<3.5	<240	1000	<280
Example52A	(48)	<4.0	6.0	<3.0	<120	750	<240
Example53A	(66)	<3.6	6.4	<3.4	<240	800	<240
Example54A	(69)	<3.8	6.8	<3.6	<300	900	<280
Example55A	(70)	<4.0	6.0	<2.8	<120	750	<240
Example56A	(72)	<3.4	5.6	<3.2	<120	750	<240
Example57A	(80)	<3.2	5.2	<3.0	<240	700	<300
Example58A	(82)	<2.8	5.0	<2.6	<100	600	<120
Example59A	(83)	<2.8	5.0	<2.4	<100	500	<100
Example60A	(84)	<3.4	6.0	<3.0	<240	880	<300
Example61A	(86)	<3.4	6.2	<3.5	<120	680	<240
Example62A	(87)	<3.0	5.6	<2.8	<100	550	<72
Example63A	(93)	<3.6	6.6	<3.4	<240	750	<340

[0147]

	TABLE 22
	Luminous Efficiency (Maximum Value)	Luminance Half-life (Maximum Value)
	Relative to Li Concentration (cd/A)	Relative to Li Concentration (h)
	Compound	Less than		More then	Less than		More than
	No.	0.05 wt %	0.05˜1.5 wt %	1.5 wt %	0.05 wt %	0.05˜1.5 wt %	1.5 wt %
Example64A	(108)	<4.0	7.0	<3.6	<400	1100	<350
Example65A	(109)	<3.5	6.0	<3.5	<360	1000	<240
Example66A	(119)	<3.0	5.6	<3.0	<260	950	<200
Example67A	(121)	<2.5	5.0	<2.8	<180	720	<240
Example68A	(124)	<3.5	8.0	<3.8	<400	1400	<550
Example69A	(127)	<4.2	9.0	<4.5	<450	1500	<600
Example70A	(130)	<4.0	7.0	<4.0	<350	1000	<400
Example71A	(133)	<3.5	6.4	<3.2	<240	850	<300
Example72A	(135)	<3.2	5.8	<3.0	<240	720	<240
Example73A	(140)	<3.0	5.5	<3.2	<200	600	<240
Example74A	(142)	<2.8	5.0	<3.0	<120	580	<240
Example75A	(143)	<3.4	6.0	<3.0	<240	720	<240
Example76A	(144)	<3.0	5.8	<2.5	<240	600	<180
Example77A	(146)	<3.5	6.5	<3.4	<300	850	<350
Example78A	(149)	<4.2	9.0	<4.8	<500	1450	<480
Example79A	(150)	<3.5	7.4	<3.8	<360	1100	<500
Example80A	(165)	<3.2	6.5	<2.8	<240	870	<450
Example81A	(168)	<3.5	7.2	<3.2	<300	1000	<500
Example82A	(182)	<3.5	6.0	<3.4	<240	900	<350
Example83A	(186)	<3.0	6.5	<2.8	<240	800	<300
Example84A	(193)	<2.5	5.0	<2.8	<180	640	<240

[0148]

	TABLE 23
	Luminous Efficiency (Maximum Value)	Luminance Half-life (Maximum Value)
	Relative to Li Concentration (cd/A)	Relative to Li Concentration (h)
	Compound	Less than		More than	Less than		More than
	No.	0.05 wt %	0.05˜1.5 wt %	1.5 wt %	0.05 wt %	0.05˜1.5 wt %	1.5 wt %
Example85A	(1)	<4.7	9.5	<3.6	<500	1480	<480
Example86A	(4)	<5.0	9.5	<3.0	<400	1200	<450
Example87A	(19)	<4.0	7.5	<3.0	<360	1100	<400
Example88A	(22)	<4.5	8.0	<3.0	<300	1000	<360
Example89A	(25)	<5.0	9.0	<3.5	<400	1200	<400
Example90A	(48)	<4.0	7.0	<3.0	<240	900	<300
Example91A	(66)	<3.2	6.0	<3.0	<240	840	<300
Example92A	(69)	<3.5	6.5	<3.5	<300	900	<450
Example93A	(80)	<3.0	6.2	<3.4	<240	840	<280
Example94A	(82)	<2.5	5.0	<3.0	<180	720	<200
Example95A	(83)	<3.5	6.0	<3.0	<240	840	<300
Example96A	(84)	<3.2	6.2	<3.5	<360	900	<350
Example97A	(108)	<3.4	6.6	<3.8	<400	950	<400
Example98A	(124)	<4.3	8.5	<4.0	<450	1150	<550
Example99A	(127)	<4.5	9.0	<4.2	<500	1400	<600
Example100A	(130)	<4.0	7.5	<3.5	<380	1000	<400
Example101A	(140)	<3.6	6.0	<3.2	<300	800	<240
Example102A	(146)	<3.6	6.0	<3.5	<240	720	<240
Example103A	(149)	<3.6	5.5	<3.2	<240	600	<200
Example104A	(182)	<3.4	6.0	<3.0	<300	900	<450
Example105A	(186)	<3.2	5.8	<2.8	<240	680	<200

[0149]

	TABLE 24
	Luminous Efficiency (Maximum Value)	Luminance Half-life (Maximum Value)
	Relative to Li Concentration (cd/A)	Relative to Li Concentration (h)
	Compound	Less than		More than	Less than		More than
	No.	0.05 wt %	0.05˜1.5 wt %	1.5 wt %	0.05 wt %	0.05˜1.5 wt %	1.5 wt %
Example106A	(1)	<4.8	9.8	<4.5	<580	1680	<400
Example107A	(4)	<5.0	10.2	<5.3	<360	1650	<450
Example108A	(5)	<4.6	8.5	<4.2	<300	1500	<400
Example109A	(19)	<4.0	8.0	<3.8	<300	1250	<360
Example110A	(108)	<3.5	6.8	<3.2	<240	960	<300
Example111A	(109)	<3.0	6.0	<3.0	<240	900	<240
Example112A	(124)	<4.6	8.0	<4.0	<300	1350	<480
Example113A	(127)	<5.2	10.5	<5.0	<450	1650	<720
Example114A	(130)	<4.3	8.5	<4.5	<380	1250	<500
Example115A	(133)	<4.0	7.8	<4.2	<380	1100	<420
Example116A	(137)	<3.5	5.8	<2.9	<240	680	<300
Example117A	(179)	<3.2	6.5	<3.4	<300	840	<420
Example118A	(182)	<4.5	8.5	<4.8	<480	1150	<480
Example119A	(184)	<3.0	6.2	<3.5	<240	720	<240
Example120A	(185)	<3.4	4.2	<3.2	<180	580	<240
Example121A	(186)	<4.2	7.2	<4.1	<380	950	<400
Example122A	(187)	<3.8	6.0	<3.2	<200	640	<180
Example123A	(188)	<3.5	5.0	<2.8	<180	550	<240
Example124A	(189)	<4.2	5.5	<3.2	<240	600	<300
Example125A	(192)	<3.8	4.8	<3.5	<100	500	<120
Example126A	(193)	<3.0	6.0	<2.8	<240	720	<200

EXAMPLE 1B

[0150] FIG. 1 is a schematic cross-sectional view illustrating the structure of an organic thin-film EL device according to a first embodiment of the present invention, wherein an organic thin-film layer contiguous to a cathode 17 is an emitter layer 15. Example 1B of the present invention will next be described with reference to FIG. 1.

[0151] On a glass substrate 11, a film of ITO (indium tin oxide) was formed by the ion plating method. The film 4, was etched into short strips, whereby the glass substrate with an anode 12 was formed. The anode 12 made of ITO had a sheet resistance of 13 Ω/□.

[0152] All the organic thin films over the ITO-adhered glass substrate were formed by the molecular-beam deposition method and the vacuum degree during film formation was set at 2×10−8 Torr or less. At an evaporation rate of 0.05 nm/s, a hole injection layer 13 made of tris(4-(4′-(N,N-di(4-tolyl)amino)styryl) phenyltriphenylamine) (which will hereinafter be abbreviated as “TTPA”) was formed to a thickness of 35 nm, followed by the formation of a hole transport layer 14 made of N,N′-diphenyl-N,N′-bis(α-naphthyl)-1,1′-biphenyl-4,4′-diamine (which will hereinafter be abbreviated as “α-NPD”) was formed to a thickness of 25 nm at an evaporation rate of 0.25 nm/s.

[0153] Over the hole transport layer, an emitter layer 15 was formed by the co-deposition method, that is, by evaporating Compound (1) in Table 1 and diphenyl 3,9-perylenedicarboxylate from different deposition sources, respectively. At that time, the evaporation rate was precisely controlled so that the diphenyl 3,9-perylenedicarboxylate was contained in the emitter layer in an amount of 3 mole %, whereby the emitter layer 15 having a thickness of 70 nm was formed.

[0154] Over the emitter layer, a cathode 17 made of a magnesium-lithium alloy was pattern formed to a thickness of 150 nm by the co-deposition method in which magnesium and lithium were evaporated from different evaporation sources respectively.

[0155] Lastly, the device was sealed in an Ar gas atmosphere. Incidentally, the concentration of lithium in the cathode 17 employed in this example was determined by the inductively coupled plasma emission spectrometry (ICP-AES).

[0156] The organic thin-film EL device was electrified and luminous efficiency and lifetime properties (luminance half-life) were evaluated. The luminous efficiency (cd/A) was found from a current density at the time when luminance of 300 cd/m2 was emitted. Lifetime properties were evaluated by causing the light emission of the device by the pulse operation at a pulse frequency of 100 Hz, duty ratio of 50% and peak current density of 10 mA/cm2. While the pulse was off, reverse bias voltage of −10V was applied.

[0157] FIG. 13 is a graph illustrating the luminous efficiency (&Circlesolid;) and luminance half-life (◯) of the cathode 17 as a function of its lithium concentration. The luminous efficiency varies with the lithium concentration of the cathode 17 and becomes 3.0 to 6.1 cd/A at a concentration range of 0.03 to 1.7 wt. %. Particularly within a concentration range of 0.03 to 1.0 wt. %, the luminous efficiency shows a stable value not less than about 5 cd/A. The luminance half-life exceeds 500 hours within a concentration range of 0.03 to 1.7 wt. %. At a concentration range less than 0.03 wt. % or greater than 1.7 wt. %, not only luminous efficiency shows a marked decrease but also luminance half-life is considerably short and does not reach even 100 hours.

[0158] The adhesion of the cathode 17 was measured by peeling in the crosshatching test. The cathode 17 having a lithium concentration of 0.03 to 1.7 wt. % showed the highest load of 1350 to 1750 gf/24 mm, while that having a lithium concentration less than 0.03 wt. % showed the load of 550 gf/24 mm or less and that having a lithium concentration greater than 1.7 wt. % showed the load of 750 gf/24 mm or less.

[0159] In this example, when the lithium concentration of the magnesium alloy cathode 17 ranges from 0.03 to 1.7 wt. %, good properties were attained and particularly at a lithium concentration of 0.03 to 1.0 wt. %, high efficiency and stable lifetime properties were attained. This result suggests that an organic thin-film EL device having excellent properties can be obtained by incorporating Compound (1) in the thin-film emitter layer 15 contiguous to the magnesium-lithium cathode 17 and setting the lithium concentration in the cathode 17 at a range of 0.03 to 1.7 wt. %, preferably 0.03 to 1.0 wt. %.

EXAMPLES 2B TO 42B)

[0160] In each of Examples 2B to 42B, except that the emitter layer 15 having a thickness of 70 nm was formed by co-deposition method in which each of the compounds shown in Tables 25 and 26 as a compound of the formula (I) and diphenyl 3, 9-perylenedicarboxylate were evaporated from different deposition sources, respectively, wherein the evaporation rate was precisely controlled so that the diphenyl 3, 9-perylenedicarboxy-late was contained in the emitter layer 15 in an amount of 3 mole %, an organic thin-film EL device was formed in a similar manner to Example 1B, and its properties were evaluated. The results are shown in Tables 25 and 26.

[0161] Even if any one of the above-described compounds was employed for the emitter layer 15, when the magnesium-lithium alloy cathode 17 had a lithium concentration ranging from 0.03 to 1.7 wt. %, luminous efficiency became about twice and luminance half-life became about three to ten times when compared with those at a lithium concentration less than 0.03 wt. % or greater than 1.7 wt. %. This suggests that when the compound represented by the formula (I) is used for an emitter layer 15 contiguous to the cathode 17, excellent advantages can be obtained at a lithium concentration adjusted to 0.03 to 1.7 wt. %.

[0162] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. The cathode 17 having a lithium concentration of 0.03 to 1.7 wt. % showed the highest load of 1200 to 1800 gf/24 mm, while that J having a lithium concentration less than 0.03 wt. % showed the load of 450 gf/24 mm or less and that having a lithium concentration greater than 1.7 wt. % showed the load of 800 gf/24 mm or less.

[0163] The above results indicate that when the compound of the formula (I) is used for an emitter layer 15 contiguous to the cathode 17, improved adhesion, high efficiency and long-life light emission can be attained by adjusting the lithium concentration in the magnesium-lithium alloy cathode 17 at 0.03 to 1.7 wt. %.

COMPARATIVE EXAMPLE 1B

[0164] Except that the emitter layer 15 having a thickness of 70 nm was formed by a co-deposition method in which conventionally and ordinarily used Alq and diphenyl 3, 9-perylenedicarboxylate were evaporated from different deposition sources, respectively, wherein the evaporation rate was precisely controlled so that the diphenyl 3, 9-perylenedicarboxylate was contained in the emitter layer 15 in an amount of 3 mole %, an organic thin-film EL device was formed in a similar manner to Example 1B, and its properties were evaluated.

[0165] As a result, it was observed, as illustrated in FIG. 17, that luminous efficiency and lifetime properties each showed a peak at a lithium concentration range exceeding 1.7 wt. %. Such a high lithium concentration range is not however preferred, because corrosion or black spots tend to appear on the electrode.

[0166] When the adhesion of the cathode portion was measured by peeling in the crosshatching test. As a result, the load was 1000 to 1200 gf/24 mm and showed the highest value when the cathode 17 having a lithium concentration exceeding 1.7 wt. % was employed, while it was 900 gf/24 mm or less when the cathode 17 having a lithium concentration less than 1.7 wt. % was employed.

EXAMPLE 43B

[0167] FIG. 2 is a schematic cross-sectional view illustrating the structure of an organic thin-film EL device according to a second embodiment of the present invention, wherein an organic thin film contiguous to a cathode 17 is an electron injection transport layer 16a and functions of an emitter layer 15 and electron injection transport layer 16a are essentially separated.

[0168] Example 43B of the present invention will next be described with reference to FIG. 2. On a glass substrate 11, an ITO (indium tin oxide) film was formed by the ion plating method, followed by etching into short strips, whereby a glass substrate with an anode 12 was formed. The anode 12 made of ITO had a sheet resistance of 13 Ω/□. Organic thin films over the ITO-applied glass substrate were all formed by the molecular-beam deposition method and the vacuum degree during the film formation was set at 2×10−8 Torr or less.

[0169] A hole injection layer 13 made of TTPA was then formed to a thickness of 35 nm at an evaporation rate of 0.05 nm/s, followed by the formation of a hole transport layer 14 made of α-NPD to a thickness of 15 nm at an evaporation rate of 0.25 nm/s.

[0170] Over the hole transport layer, an emitter layer 15 made of 9,10-bis(4-(4-(N,N-di(4-tolyl)aminophenyl) benzyliden)anthracene (which will hereinafter be abbreviated as “BPBA”) was formed to a thickness of 48 nm at an evaporation rate of 0.07 nm/s.

[0171] Over the emitter layer 15, an electron injection transport layer 16a made of the compound (1) in Table 1 was formed to a thickness of 35 nm at an evaporation rate of 0.2 nm/s.

[0172] Then, a cathode 17 made of a magnesium-lithium alloy was pattern-formed to a thickness of 150 nm over the electron injection transport layer by the co-deposition method in which magnesium and lithium were evaporated from different evaporation sources, respectively.

[0173] Finally, the resulting device was sealed in an Ar gas atmosphere. In Example 43B, the concentration of lithium in the cathode 17 was determined by ICP-AES.

[0174] The organic thin film EL device so formed was electrified and luminous efficiency and lifetime properties (luminance half-life) were evaluated. The luminous efficiency (cd/A) was found from a current density at the time when luminance of 300 cd/m2 was emitted. Lifetime properties were evaluated by causing the light emission of the device by the pulse operation at a pulse frequency of 100 Hz, duty ratio of 50% and peak current density of 10 mA/cm2. While the pulse was off, reverse bias voltage of −10V was applied.

[0175] FIG. 14 is a graph illustrating the luminous efficiency (&Circlesolid;) and luminance half-life (◯) of the cathode 17 as a function of its lithium concentration. The luminous efficiency varies with the lithium concentration of the cathode 17 and becomes 5.5 to 7.1 cd/A at a concentration range of 0.03 to 1.7 wt. %. The luminance half-life exceeded 400 hours within a concentration range of 0.03 to 1.7 wt. %. At a concentration outside the above range, that is, a range less than 0.03 wt. % or greater than 1.7 wt. %, luminous efficiency decreased to about half of that within the above range and luminance half-life became even as short as 120 hours or less.

[0176] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. The cathode 17 having a lithium concentration of 0.03 to 1.7 wt. % showed the highest load of 1500 to 1800 gf/24 mm, while that having a lithium concentration less than 0.03 wt. % showed the load of 550 gf/24 mm or less and that having a lithium concentration greater than 1.7 wt. % showed the load of 850 gf/24 mm or less.

[0177] In this Example 43B, when the lithium concentration in the magnesium alloy cathode 17 falls within a range of 0.03 to 1.7 wt. %, good properties were attained. This result suggests that, with respect to organic thin-film EL devices having the device structure shown in FIG. 2, an organic thin-film EL device having excellent properties can be obtained by incorporating Compound (1) of Table 1 in the electron injection transport layer 16a contiguous to the cathode 17 made of a magnesium-lithium alloy and setting the lithium concentration range in the cathode 17 at 0.03 to 1.7 wt. %.

EXAMPLES 44B TO 84B

[0178] In each of Examples 44B to 84B, in a similar manner to Example 43B except that each of the compounds shown in Tables 27 and 28 was used as the compound of the formula (I) for forming the electron injection transport layer 16 a of FIG. 2, an organic thin-film EL device was formed and its properties were evaluated. Results are shown in Tables 27 and 28.

[0179] Even if any one of the above-described compounds were employed as the hole injection transport layer 16a, when the magnesium-lithium alloy cathode 17 had a lithium concentration ranging from 0.03 to 1.7 wt. %, luminous efficiency became about twice and luminance half-life became about three to ten times when compared with those at a lithium concentration less than 0.03 wt. % or greater than 1.7 wt. %. This suggests that when the compound represented by the formula (I) is used for the electron injection transport layer 16a contiguous to the magnesium-lithium alloy cathode 17, excellent advantages can be obtained at a lithium concentration adjusted to 0.03 to 1.7 wt. %.

[0180] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. The cathode 17 having a lithium concentration of 0.03 to 1.7 wt. % showed the highest load of 1200 to 1800 gf/24 mm, while that having a lithium concentration less than 0.03 wt. % showed the load of 550 gf/24 mm or less and that having a lithium concentration greater than 1.7 wt. % showed the load of 850 gf/24 mm or less.

[0181] The above results suggest that when the compound of the formula (I) is used for the electron injection transport layer 16a contiguous to the cathode 17, improved adhesion, high efficiency and long-life light emission can be attained by adjusting the lithium concentration in the cathode 17 made of a magnesium-lithium alloy at 0.03 to 1.7 wt. %.

COMPARATIVE EXAMPLE 2B

[0182] In a similar manner to Example 43B except that conventionally and ordinarily used Alq was used for the formation of the electron injection transport layer 16a, an organic thin-film EL device was formed and its properties were evaluated. As a result, it was observed, as illustrated in FIG. 18, that luminous efficiency and lifetime properties each showed a peak in a range of the lithium concentration exceeding 1.7 wt. %. Such a high lithium concentration range is not preferred because corrosion or black spots tend to appear.

[0183] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. As a result, the load was 1000 to 1200 gf/24 mm and showed the highest value when the cathode 17 having a lithium concentration exceeding 1.7 wt. % was employed, while it was 900 gf/24 mm or less when the cathode 17 having a lithium concentration not greater than 1.7 wt. % was employed.

EXAMPLE 85B

[0184] FIG. 3 is a schematic cross-sectional view illustrating the structure of an organic thin-film EL device according to a third embodiment of the present invention, which is different from the structure of the second embodiment in that at least one of the cathode components is contained in the electron injection transport layer 16b contiguous to the cathode 17.

[0185] Example 85B of the present invention will next be described with reference to FIG. 3. On a glass substrate 11, an ITO (indium tin oxide) film was formed by the ion plating method, followed by etching into short strips, whereby a glass substrate with an anode 12 was formed. The anode 12 made of ITO had a sheet resistance of 13 Ω/□. The organic thin films over the ITO-applied glass substrate were all formed by the molecular-beam deposition method and the vacuum degree during the film formation was set at 2×10−8 Torr or less.

[0186] A hole injection layer 13 made of TTPA was then formed to a thickness of 35 nm at an evaporation rate of 0.05 nm/s, followed by the formation of a hole transport layer 14 made of α-NPD to a thickness of 25 nm at an evaporation rate of 0.25 nm/s.

[0187] Over the hole transport layer, an emitter layer 15 made of BPBA was formed to a thickness of 48 nm at an evaporation rate of 0.07 nm/s. Over the emitter layer 15, an electron injection transport layer 16b containing 1.5 wt. % of lithium was formed to a thickness of 35 nm by the co-deposition method in which lithium and the compound (1) were evaporated as electron transport materials from different evaporation sources, respectively.

[0188] Then, a cathode 17 made of a magnesium-lithium alloy was pattern-formed to a thickness of 150 nm over the electron injection transport layer by the co-deposition method in which magnesium and lithium were evaporated from different evaporation sources respectively.

[0189] Finally, the resulting device was sealed in an Ar gas atmosphere. In this Example 85B, the concentration of lithium in the cathode 17 was determined by ICP-AES.

[0190] FIG. 15 is a graph illustrating the luminous efficiency (&Circlesolid;) and luminance half-life (◯) of the cathode 17 as a function of its lithium concentration. The luminous efficiency varies with the lithium concentration of the cathode 17 and became 6.4 to 8.4 cd/A in a concentration range of 0.03 to 1.7 wt. %. The luminance half-life was not less than 440 hours within a concentration range of 0.03 to 1.7 wt. %. At a concentration outside the above range, that is, a range of less than 0.03 wt. % or greater than 1.7 wt. %, not only luminous efficiency but also luminance half-life decreased to half or less of that within the above range and luminance half-life became even 120 hours or less. In addition, in this Example 85B, the luminous efficiency and lifetime properties were improved by about 10 to 20% when compared with those of Example 43B. Such an improvement in the properties was brought about by doping 14 lithium, which is one of the cathode components, into the electron injection transport layer 16b of the organic thin-film EL device of the present invention.

[0191] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. The cathode 17 having a lithium concentration of 0.03 to 1.7 wt. % showed the highest load of 1750 to 2150 gf/24 mm, while that having a lithium concentration less than 0.03 wt. % showed the load of 900 gf/24 mm and that having a lithium concentration greater than 1.7 wt. % showed the load of 1100 gf/24 mm. The adhesion was improved by 1.2 times when compared with that in Example 43B. Such an improvement in the properties was brought about by doping lithium, which is one of the cathode components, into the electron injection transport layer 16b of the present invention, thereby improving the adhesion.

[0192] In this Example, when the magnesium alloy cathode 17 had a lithium concentration of 0.03 to 1.7 wt. %, properties were good. This result suggests that, with respect to organic thin-film EL devices having the device structure shown in FIG. 3, an organic thin film EL device having excellent properties can be obtained by incorporating Compound (1) in the electron injection transport layer 16b contiguous to the cathode 17 made of a magnesium-lithium alloy and setting the lithium concentration in the cathode 17 at 0.03 to 1.7 wt.

EXAMPLES 86B TO 105B

[0193] In each of Examples 86B to 105B, in a similar manner to Example 85B except that each of the compounds shown in Tables 29 was used for the electron injection transport layer 16b of FIG. 3, an organic thin-film EL device was formed and its properties were evaluated. Results are shown in Tables 29.

[0194] Even if any one of the above-described compounds were employed as the electron injection transport layer 16b, when the magnesium-lithium alloy cathode 17 had a lithium concentration ranging from 0.03 to 1.7 wt. %, luminous efficiency became about twice and luminance half-life became about three to nine times when compared with those at a lithium concentration less than 0.03 wt. % or greater than 1.7 wt. %. This suggests that when the compound represented by the formula (I) is used for the electron injection transport layer 16b contiguous to the cathode 17 of the organic thin-film EL device illustrated in FIG. 3, excellent advantages can be obtained at a lithium concentration adjusted to 0.03 to 1.7 wt. %.

[0195] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. The cathode 17 having a lithium concentration of 0.03 to 1.7 wt. % showed the highest load of 1750 to 2150 gf/24 mm, while that having a lithium concentration less than 0.03 wt. % showed the load of 900 gf/24 mm or less and that having a lithium concentration greater than 1.7 wt. % showed the load of 1100 gf/24 mm or less.

[0196] The above results suggest that when the compound of the formula (I) is used for the electron injection transport layer 16b contiguous to the cathode 17, improved adhesion, high efficiency and long-life light emission can be attained by adjusting the lithium concentration in the cathode 17 made of an magnesium-lithium alloy at 0.03 to 1.7 wt. %.

COMPARATIVE EXAMPLE 3B

[0197] In a similar manner to Example 85B except that the electron injection transport layer 16b was formed by doping lithium into a layer composed of conventionally and ordinarily used Alq, an organic thin-film EL device was formed and its properties were evaluated. As a result, it was observed, as illustrated in FIG. 19, that luminous efficiency and lifetime properties each showed a peak in a range of the lithium concentration exceeding 1.7 wt %.

[0198] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. As a result, the load was 1000 to 1200 gf/24 mm and showed the highest value when the cathode 17 having a lithium concentration exceeding 1.7 wt. % was employed, while it was 900 gf/24 mm or less when the cathode 17 having a lithium concentration not greater than 1.7 wt. % was employed.

EXAMPLE 106B

[0199] FIG. 4 is a schematic cross-sectional view illustrating the structure of an organic thin-film EL device according to a fourth embodiment of the present invention, which is different from the structures of the other embodiments in that a cathode protective layer 18 is disposed over a cathode 17.

[0200] Example 106B of the present invention will next be described with reference to FIG. 4. On a glass substrate 11, an ITO (indium tin oxide) film was formed by the ion plating method, followed by etching into short strips, whereby a glass substrate with an anode 12 was formed. The anode 12 made of ITO had a sheet resistance of 13 Ω/□. Organic thin films over the ITO-applied glass substrate were all formed by the molecular-beam deposition method and the vacuum degree during the film formation was set at 2×10−8 Torr or less.

[0201] A hole injection layer 13 made of TTPA was then formed to a thickness of 35 nm at an evaporation rate of 0.05 nm/s, followed by the formation of a hole transport layer 14 made of α-NPD to a thickness of 15 nm at an evaporation rate of 0.25 nm/s.

[0202] Over the hole transport layer, an emitter layer 15 made of BPBA was formed to a thickness of 48 nm at an evaporation rate of 0.07 nm/s. Over the emitter layer 15, an electron injection transport layer 16a composed of the compound (1) was formed to a thickness of 35 nm at an evaporation rate of 0.2 nm/s.

[0203] Over the electron injection transport layer, a cathode 17 made of a magnesium-lithium alloy was pattern-formed to a thickness of 30 nm by the co-deposition method in which magnesium and lithium were evaporated from different evaporation sources respectively.

[0204] Over the cathode, an aluminum-scandium alloy was formed to a thickness of 300 nm as a protective layer 18 for the cathode 17 by the RF sputtering method.

[0205] Finally, the resulting device was sealed in an Ar gas atmosphere. In this Example 106B, the concentration of lithium in the cathode 17 was determined by ICP-AES.

[0206] FIG. 16 is a graph illustrating the luminous efficiency (&Circlesolid;) and luminance half-life (◯) of the cathode 17 as a function of its lithium concentration. The luminous efficiency varies with the lithium concentration of the cathode 17 and becomes 5.0 to 7.1 cd/A at a concentration range of 0.03 to 1.7 wt. %. The luminance half-life exceeds 700 hours within a concentration range of 0.03 to 1.7 wt. % and above all, it exceeds 1000 hours at a concentration range of 0.4 to 1.0 wt. %. At a concentration outside the above range, that is, at a concentration less than 0.03 wt. % or greater than 1.7 wt. %, on the other hand, not only the luminous efficiency decreases to half or less than that within the above range but also luminance half-life decreases even as short as 100 hours or less.

[0207] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. The cathode 17 having a lithium concentration of 0.03 to 1.7 wt. % showed the highest load of 1500 to 1800 gf/24 mm, while that having a lithium concentration less than 0.03 wt. % showed the load of 550 gf/24 mm and that having a lithium concentration greater than 1.7 wt. % showed the load of 850 gf/24 mm.

[0208] In this Example, when the magnesium alloy cathode 17 had a lithium concentration of 0.03 to 1.7 wt. %, properties were good and particularly at a lithium concentration of 0.4 to 1.0 wt. %, luminous efficiency was high and lifetime properties were stable. This result suggests that, with respect to organic thin-film EL devices having the device structure shown in FIG. 4, an organic thin-film EL device having excellent properties can be obtained by incorporating the Compound (1) in the electron injection transport layer 16a contiguous to the cathode 17 made of a magnesium and lithium alloy and setting the lithium concentration in the cathode 17 at a range of 0.03 to 1.7 wt. %, preferably 0.4 to 1.0 wt. %.

EXAMPLES 107B TO 126B

[0209] In each of Examples 107B to 126B, in a similar manner to Example 106B except that each of the compounds shown in Tables 30 was used for the electron injection transport layer 16a of FIG. 4, an organic thin-film EL device was formed and its properties were evaluated. The results are shown in Tables 30.

[0210] Even if any one of the above-described compounds were employed as the electron injection transport layer 16a, when the magnesium-lithium alloy cathode 17 had a lithium concentration ranging from 0.03 to 1.7 wt. %, luminous efficiency became about twice and luminance half-life became about three to four times when compared with those at a lithium concentration less than 0.03 wt. % or greater than 1.7 wt. %.

[0211] This suggests that, with respect to organic thin-film EL devices having the device structure shown in FIG. 4, when the compound represented by the formula (I) is used for the emitter layer 15 contiguous to the cathode 17, excellent advantages can be obtained at a lithium concentration adjusted to 0.03 to 1.7 wt. %. The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. The cathode 17 having a lithium concentration of 0.05 to 1.5 wt. % showed the highest load of 1500 to 1800 gf/24 mm, while that having a lithium concentration less than 0.05 wt. % showed the load of 550 gf/24 mm or less and that having a lithium concentration greater than 1.5 wt. % showed the load of 850 gf/24 mm or less.

[0212] The above results suggest that when the compound of the formula (I) is used for the electron injection transport layer 16a contiguous to the cathode 17, an improvement in adhesion is brought about by adjusting the lithium concentration in the magnesium-lithium alloy cathode 17 at 0.03 to 1.7 wt. % and at the same time, high efficiency and long-life light emission can be attained by disposing the cathode protective layer 18 over the cathode 17.

COMPARATIVE EXAMPLE 4B

[0213] In a similar manner to Example 106B except that the electron injection transport layer 16a was formed using the conventionally and ordinarily used Alq, an organic thin-film EL device was formed and its properties were evaluated.

[0214] As a result, it was observed, as illustrated in FIG. 20, that luminous efficiency and luminance half-life each showed a peak in a range of the lithium concentration exceeding 1.7 wt. %.

[0215] The adhesion of the cathode portion 17 was measured by peeling in the crosshatching test. As a result, the load was 1000 to 1200 gf/24 mm and showed the highest value when the cathode 17 having a lithium concentration exceeding 1.7 wt. % was employed, while it was 900 gf/24 mm when the cathode 17 having a lithium concentration not greater than 1.7 wt. % was employed.

	TABLE 25
	Luminous Efficiency (Maximum Value)	Luminance Half-life (Maximum Value)
	Relative to Li Concentration (cd/A)	Relative to Li Concentration (h)
	Compound	Less than		More than	Less than		More than
	No.	0.05 wt %	0.05˜1.5 wt %	1.5 wt %	0.05 wt %	0.05˜1.5 wt %	1.5 wt %
Example1B	(1)	<2.4	6.1	<2.8	<100	1000	<100
Example2B	(4)	<2.6	6.5	<2.8	<150	1100	<120
Example3B	(5)	<2.6	6.0	<2.6	<150	1000	<200
Example4B	(15)	<2.5	5.0	<2.5	<120	900	<150
Example5B	(17)	<2.2	4.5	<2.2	<120	840	<100
Example6B	(18)	<2.6	4.8	<2.5	<180	860	<200
Example7B	(19)	<3.0	5.0	<2.8	<240	860	<250
Example8B	(22)	<3.1	4.8	<2.8	<240	720	<200
Example9B	(25)	<3.5	6.4	<2.8	<350	1000	<300
Example10B	(26)	<3.5	6.0	<3.2	<320	950	<260
Example11B	(29)	<3.0	4.5	<3.2	<240	720	<240
Example12B	(32)	<3.2	4.8	<3.0	<300	850	<300
Example13B	(48)	<3.0	5.5	<2.8	<240	700	<200
Example14B	(62)	<3.0	5.2	<3.1	<200	750	<250
Example15B	(63)	<3.0	4.9	<2.8	<250	620	<240
Example16B	(66)	<2.5	4.8	<2.3	<220	600	<200
Example17B	(69)	<3.0	5.0	<3.2	<320	650	<280
Example18B	(70)	<2.6	5.5	<3.0	<350	740	<240
Example19B	(72)	<2.3	5.0	<2.8	<240	500	<180
Example20B	(80)	<2.4	4.5	<2.3	<200	450	<120
Example21B	(82)	<2.0	4.2	<1.8	<160	330	<120

[0216]

	TABLE 26
	Luminous Efficiency (Maximum Value)	Luminance Half-life (Maximum Value)
	Relative to Li Concentration (cd/A)	Relative to Li Concentration (h)
	Compound	Less than		More than	Less than		More than
	No.	0.05 wt %	0.05˜1.5 wt %	1.5 wt %	0.05 wt %	0.05˜1.5 wt %	1.5 wt %
Example22B	(83)	<2.2	4.6	<2.4	<100	380	<100
Example23B	(84)	<2.0	4.0	<1.8	<100	480	<240
Example24B	(86)	<2.2	4.2	<2.8	<240	580	<200
Example25B	(87)	<2.0	3.8	<1.8	<24	240	<24
Example26B	(93)	<1.6	2.8	<1.4	<72	280	<48
Example27B	(96)	<1.5	2.9	<1.6	<72	280	<72
Example28B	(107)	<1.7	3.6	<1.4	<100	500	<120
Example29B	(119)	<2.0	3.6	<1.8	<120	480	<240
Example30B	(121)	<2.0	3.2	<1.6	<72	360	<72
Example31B	(122)	<2.8	4.4	<2.2	<72	480	<120
Example32B	(124)	<3.0	5.5	<2.6	<120	600	<200
Example33B	(127)	<3.0	5.8	<3.0	<200	760	<200
Example34B	(130)	<3.0	5.6	<2.6	<120	800	<200
Example35B	(133)	<2.6	4.8	<2.8	<100	720	<180
Example36B	(140)	<2.4	4.5	<2.8	<120	600	<240
Example37B	(142)	<2.8	4.4	<2.4	<200	640	<120
Example38B	(143)	<3.1	5.4	<3.0	<320	600	<280
Example39B	(144)	<2.4	4.2	<3.1	<240	480	<100
Example40B	(146)	<3.0	5.0	<3.2	<240	600	<200
Example41B	(165)	<3.6	6.0	<3.5	<300	800	<400
Example42B	(169)	<2.8	5.2	<3.2	<240	550	<240

[0217]

	TABLE 27
	Luminous Efficiency (Maximum Value)	Luminance Half-life (Maximum Value)
	Relative to Li Concentration (cd/A)	Relative to Li Concentration (h)
	Compound	Less than		More than	Less than		More than
	No.	0.05 wt %	0.05˜1.5 wt %	1.5 wt %	0.05 wt %	0.05˜1.5 wt %	1.5 wt %
Example43B	(1)	<2.8	7.1	<2.2	<100	1200	<100
Example44B	(4)	<4.3	8.4	<4.0	<400	1150	<200
Example45B	(5)	<4.0	7.8	<4.0	<300	1100	<200
Example46B	(18)	<3.5	6.5	<3.8	<300	900	<240
Example47B	(19)	<3.8	6.2	<3.9	<320	1050	<240
Example48B	(21)	<3.4	5.0	<3.0	<240	720	<240
Example49B	(22)	<4.5	6.8	<4.0	<300	1000	<400
Example50B	(25)	<4.8	7.4	<3.5	<350	950	<400
Example51B	(26)	<4.0	6.5	<3.2	<200	900	<280
Example52B	(48)	<3.8	6.2	<2.8	<200	760	<240
Example53B	(66)	<3.8	6.8	<3.8	<300	840	<300
Example54B	(69)	<3.5	6.0	<3.0	<400	900	<480
Example55B	(70)	<4.2	5.2	<2.4	<180	720	<200
Example56B	(72)	<3.4	5.6	<3.2	<120	750	<240
Example57B	(80)	<3.0	4.8	<2.8	<200	660	<320
Example58B	(82)	<2.8	4.8	<2.6	<100	500	<120
Example59B	(83)	<3.0	5.4	<2.8	<200	600	<240
Example60B	(84)	<3.4	6.0	<3.0	<240	880	<300
Example61B	(86)	<3.4	6.2	<3.5	<120	680	<240
Example62B	(87)	<3.5	5.8	<2.8	<200	400	<48
Example63B	(93)	<3.1	6.0	<3.6	<200	720	<240

[0218]

	TABLE 28
	Luminous Efficiency (Maximum Value)	Luminance Half-life (Maximum Value)
	Relative to Li Concentration (cd/A)	Relative to Li Concentration (h)
	Compound	Less than		More than	Less than		More than
	No.	0.05 wt %	0.05˜1.5 wt %	1.5 wt %	0.05 wt %	0.05˜1.5 wt %	1.5 wt %
Example64B	(108)	<3.8	6.5	<3.4	<400	1000	<300
Example65B	(109)	<3.4	6.0	<3.5	<400	1100	<360
Example66B	(119)	<3.2	5.3	<2.8	<360	850	<400
Example67B	(121)	<2.2	4.0	<2.8	<120	600	<200
Example68B	(124)	<3.2	6.8	<3.3	<300	1100	<480
Example69B	(127)	<4.0	8.0	<4.0	<300	1250	<500
Example70B	(130)	<3.5	6.2	<3.6	<300	960	<300
Example71B	(133)	<3.5	6.0	<3.0	<200	720	<240
Example72B	(135)	<3.0	5.0	<3.1	<240	600	<200
Example73B	(140)	<3.2	6.5	<3.2	<200	700	<300
Example74B	(142)	<2.6	4.6	<3.1	<120	550	<100
Example75B	(143)	<3.0	5.2	<2.8	<200	720	<240
Example76B	(144)	<3.0	5.0	<2.8	<240	680	<200
Example77B	(146)	<3.2	6.5	<3.4	<300	850	<350
Example78B	(149)	<4.1	8.4	<4.2	<480	1250	<300
Example79B	(150)	<3.2	7.0	<3.2	<400	1000	<400
Example80B	(165)	<3.0	6.0	<2.8	<200	700	<350
Example81B	(168)	<3.5	6.5	<3.0	<300	900	<500
Example82B	(182)	<3.8	5.8	<3.1	<150	700	<240
Example83B	(186)	<3.2	6.0	<2.8	<300	720	<240
Example84B	(193)	<2.6	4.6	<2.8	<200	560	<200

[0219]

	TABLE 29
	Luminous Efficiency (Maximum Value)	Luminance Half-Life (Maximum Value)
	Relative to Li Concentration (cd/A)	Relative to Li Concentration (h)
	Compound	Less than		More than	Less than		More than
	No.	0.05 wt %	0.05˜1.5 wt %	1.5 wt %	0.05 wt %	0.05˜1.5 wt %	1.5 wt %
Example85B	(1)	<3.8	8.1	<3.2	<100	960	<400
Example86B	(4)	<4.5	8.6	<3.8	<400	1100	<380
Example87B	(19)	<4.2	7.8	<3.2	<350	1000	<420
Example88B	(22)	<4.0	7.2	<3.1	<280	960	<300
Example89B	(25)	<4.5	8.2	<3.8	<500	1000	<400
Example90B	(48)	<3.8	6.6	<2.8	<200	850	<400
Example91B	(66)	<3.2	6.0	<3.0	<240	840	<300
Example92B	(69)	<3.5	6.0	<3.0	<240	720	<300
Example93B	(80)	<3.0	6.2	<3.4	<240	840	<280
Example94B	(82)	<2.5	5.0	<3.0	<180	720	<200
Example95B	(83)	<3.0	5.2	<3.1	<400	800	<240
Example96B	(84)	<3.0	5.6	<3.1	<300	850	<380
Example97B	(108)	<3.2	6.2	<3.4	<360	800	<300
Example98B	(124)	<4.0	7.4	<3.5	<400	1100	<480
Example99B	(127)	<4.0	7.5	<4.0	<580	1250	<650
Example100B	(130)	<3.4	7.0	<3.2	<480	960	<360
Example101B	(140)	<3.8	5.2	<3.6	<200	720	<240
Example102B	(146)	<3.6	6.0	<3.5	<240	720	<240
Example103B	(149)	<3.0	5.0	<3.0	<200	580	<180
Example104B	(182)	<3.0	5.0	<3.0	<300	600	<240
Example105B	(186)	<2.8	5.2	<3.2	<280	720	<240

[0220]

	TABLE 30
	Luminous Efficiency (Maximum Value)	Luminance Half-Life (Maximum Value)
	Relative to Li Concentration (cd/A)	Relative to Li Concentration (h)
	Compound	Less than		More than	Less than		More than
	No.	0.05 wt %	0.05˜1.5 wt %	1.5 wt %	0.05 wt %	0.05˜1.5 wt %	1.5 wt %
Example106B	(1)	<4.0	7.1	<4.0	<400	1300	<400
Example107B	(4)	<4.3	8.4	<4.0	<400	1500	<400
Example108B	(5)	<4.0	7.8	<4.0	<300	1400	<400
Example109B		<3.8	6.2	<3.9	<320	1250	<260
Example110B	(108)	<3.8	6.5	<3.4	<500	1200	<400
Example111B	(109)	<3.4	6.0	<3.5	<450	1300	<400
Example112B	(124)	<3.2	6.8	<3.3	<350	1300	<600
Example113B	(127)	<4.0	8.0	<4.0	<330	1400	<600
Example114B	(130)	<3.5	6.2	<3.6	<300	1150	<350
Example115B	(133)	<3.5	6.0	<3.0	<240	800	<280
Example116B	(137)	<3.2	5.0	<2.5	<200	580	<240
Example117B	(179)	<3.0	6.0	<3.0	<280	720	<300
Example118B	(182)	<3.8	5.8	<3.1	<200	800	<300
Example119B	(184)	<2.6	5.7	<3.2	<260	680	<200
Example120B	(185)	<3.0	4.0	<3.0	<150	480	<200
Example121B	(186)	<3.2	6.0	<2.8	<350	800	<300
Example122B	(187)	<3.4	5.5	<3.0	<200	600	<200
Example123B	(188)	<3.0	4.6	<2.6	<150	480	<200
Example124B	(189)	<4.0	5.0	<3.0	<240	500	<200
Example125B	(192)	<3.5	4.5	<3.1	<100	400	<120
Example126B	(193)	<2.6	4.6	<2.8	<240	600	<240

Claims

1. An organic thin-film EL device of a charge injection type which has an organic thin-film layer contiguous to the surface of a cathode opposite to an anode, said organic thin-film layer contains an organic compound represented by the following formula (I):

2. An organic thin-film EL device of a charge injection type which has an organic thin-film layer contiguous to the surface of a cathode opposite to an anode, said organic thin-film layer contains an organic compound represented by the following formula (I):

3. An organic thin-film EL device according to claim 1, wherein the cathode has a film thickness of 1 to 50 nm and has a cathode protective layer thereon.

4. An organic thin-film EL device according to claim 2, wherein the cathode has a film thickness of 1 to 50 nm and has a cathode protective layer thereon.

5. An organic thin-film EL device according to claim 1, wherein the cathode has a film thickness of 1 to 50 nm and has a cathode protective layer thereon, said cathode protective layer comprising aluminum single substance or an aluminum alloy.

6. An organic thin-film EL device according to claim 1, wherein at least one of the components contained in the cathode has been doped into the organic thin film contiguous to said cathode.

7. An organic thin-film EL device according to claim 2, wherein at least one of the components contained in the cathode has been doped into the organic thin film contiguous to said cathode.

8. An organic thin-film EL device according to claim 3, wherein at least one of the components contained in the cathode protective layer has been doped into the organic thin film contiguous to said cathode.

9. An organic thin-film EL device according to claim 4, wherein at least one of the components contained in the cathode protective layer has been doped into the organic thin film contiguous to said cathode.

10. An organic thin-film EL device according to claim 5, wherein at least one of the components contained in the cathode protective layer has been doped into the organic thin film contiguous to said cathode.

11. An organic thin-film EL device according to claim 1, wherein the organic thin film layer contiguous to the cathode is an emitter layer.

12. An organic thin-film EL device according to claim 2, wherein the organic thin film layer contiguous to the cathode is an emitter layer.

13. An organic thin-film EL device according to claim 3, wherein the organic thin film layer contiguous to the cathode is an emitter layer.

14. An organic thin-film EL device according to claim 4, wherein the organic thin film layer contiguous to the cathode is an emitter layer.

15. An organic thin-film EL device according to claim 5, wherein the organic thin film layer contiguous to the cathode is an emitter layer.

16. An organic thin-film EL device according to claim 6, wherein the organic thin film layer contiguous to the cathode is an emitter layer.

17. An organic thin-film EL device according to claim 7, wherein the organic thin film layer contiguous to the cathode is an emitter layer.

18. An organic thin-film EL device according to claim 8, wherein the organic thin film layer contiguous to the cathode is an emitter layer.

19. An organic thin-film EL device according to claim 9, wherein the organic thin film layer contiguous to the cathode is an emitter layer.

20. An organic thin-film EL device according to claim 10, wherein the organic thin film layer contiguous to the cathode is an emitter layer.

21. An organic thin-film EL device according to claim 1, wherein the organic thin film layer contiguous to the cathode is an electron injection transport layer.

22. An organic thin-film EL device according to claim 2, wherein the organic thin film layer contiguous to the cathode is an electron injection transport layer.

23. An organic thin-film EL device according to claim 3, wherein the organic thin film layer contiguous to the cathode is an electron injection transport layer.

24. An organic thin-film EL device according to claim 4, wherein the organic thin film layer contiguous to the cathode is an electron injection transport layer.

25. An organic thin-film EL device according to claim 5, wherein the organic thin film layer contiguous to the cathode is an electron injection transport layer.

26. An organic thin-film EL device according to claim 6, wherein the organic thin film layer contiguous to the cathode is an electron injection transport layer.

27. An organic thin-film EL device according to claim 71 wherein the organic thin film layer contiguous to the cathode is an electron injection transport layer.

28. An organic thin-film EL device according to claim 8, wherein the organic thin film layer contiguous to the cathode is an electron injection transport layer.

29. An organic thin-film EL device according to claim 9, wherein the organic thin film layer contiguous to the cathode is an electron injection transport layer.

30. An organic thin-film EL device according to claim 10, wherein the organic thin film layer contiguous to the cathode is an electron injection transport layer.