Lithium cobalt oxides and methods of making same

Abstract

The present invention includes lithium cobalt oxides having hexagonal layered crystal structures and methods of making same. The lithium cobalt oxides of the invention have the formula LiwCo1−xAxO2+y wherein 0.96≦w≦1.05, 0≦x≦0.05,

Description

FIELD OF THE INVENTION

[0002] The present invention relates to lithium cobalt oxides for use as positive electrode materials for rechargeable lithium and lithium-ion secondary batteries, and to methods of making lithium cobalt oxides.

BACKGROUND OF THE INVENTION

[0003] LiCoO2 is currently being used in over 95% of commercial lithium and lithium-ion secondary batteries as the active positive electrode material. The current production rate of lithium and lithium-ion batteries is about 30 million units per month with each unit containing about 10-15 g of LiCoO2 (i.e., 300-450 metric tons/month).

[0004] LiCoO2 can be made by a number of different methods by reacting a lithium salt and a cobalt salt. However, these methods often involve lengthy reaction times thereby reducing the rate of LiCoO2 production.

[0005] Therefore, there is a need in the art to provide a method of preparing LiCoO2 that demonstrates good performance in rechargeable lithium and lithium-ion secondary batteries and that can be produced with a relatively short reaction time.

SUMMARY OF THE INVENTION

[0006] The present invention includes lithium cobalt oxides having hexagonal layered crystal structures and methods of making same. The lithium cobalt oxides of the invention have the formula LiwCo1−xAxO2+y wherein 0.96≦w≦1.05, 0≦x≦0.05,

[0007] −0.02≦y≦0.02 and A is one or more dopants. Preferably, 0.98≦w≦1.02 and 0≦x≦0.02.

[0008] The lithium cobalt oxides of the invention preferably have a position within the principal component space defined by the following relationship:

ax i +by i ≦c

[0009] wherein xi={right arrow over (S)}i·{right arrow over (P)}c1; yi={right arrow over (S)}i·{right arrow over (P)}c2; the vector {right arrow over (S)}i is the x-ray spectrum for the LiwCo1−xAxO2+y compound; the vectors {right arrow over (P)}c1 and {right arrow over (P)}c2 are determined by measuring the x-ray powder diffraction values {right arrow over (S)}i between 15° and 120° using a 0.02° step size and CuKα rays for a large sample set of lithium cobalt oxides and using the regression of {right arrow over (S)}i of the sample set against the capacity fade after 50 cycles of a lithium coin cell that includes a lithium negative electrode and the lithium cobalt oxide as the positive electrode material and that is cycled between 3.0 and 4.3V at a constant current of C/3 during both charge and discharge cycles; and the values a, b and c are determined by using only the xi and yi values for LiwCo1−xAxO2+y compounds in the sample set that have a capacity fade after 50 cycles of less than or equal to 15%.

[0010] More preferably, the lithium cobalt oxides of the invention have a position within the principal component space defined by the following relationship:

x i +0.77yi≦−6

[0011] wherein xi={right arrow over (S)}i·{right arrow over (P)}c1; yi={right arrow over (S)}i·{right arrow over (P)}c2; {right arrow over (S)}i is the x-ray spectrum for the LiwCo1−xAxO2+y compound; and {right arrow over (P)}c1 and {right arrow over (P)}c2 are determined by measuring the x-ray powder diffraction values {right arrow over (S)}i between 15° and 120° using a 0.02° step size and CuKα rays for a large sample set of lithium cobalt oxides and using the partial least squares regression (PLSR) of {right arrow over (S)}i of the sample set against the capacity fade after 50 cycles of a lithium coin cell that includes a lithium negative electrode and the lithium cobalt oxide as the positive electrode material and that is cycled between 3.0 and 4.3V at a constant current of C/3 during both charge and discharge cycles. For example, {right arrow over (P)}c1 and {right arrow over (P)}c2 can be defined by the coefficients provided in Table 1 (wherein 2θ is the scattering angle of x-ray powder diffraction measurements using CuKα rays).

[0012] The lithium cobalt oxides of the invention can be used in the positive electrode of a rechargeable lithium or lithium-ion secondary battery in accordance with the invention. For the lithium cobalt oxides of the invention, the capacity fade of a lithium coin cell having a lithium negative electrode and using the lithium cobalt oxide as the positive electrode material when cycled between 3.0 and 4.3V at a constant current of C/3 during both charge and discharge cycles after 50 charge/discharge cycles is preferably less than or equal to 15%, more preferably less than or equal to 10%. Moreover, the initial specific discharge capacity is preferably greater than or equal to 154 mAh/g.

[0013] The lithium cobalt oxides of the invention are prepared by heating a lithium source compound, a cobalt source compound and optionally one or more source compounds that include dopants A at a temperature below about 850° C. to produce LiwCo1−xAxO2+y and heating the LiwCo1−xAxO2+y compound at a temperature from about 900° C. and 1000° C. to form and enhance the hexagonal layered crystal structure of the LiwCo1−xAxO2+y compound. The temperature in the first heating step is preferably from about 500° C. to about 850° C. and the temperature in the second heating step is preferably from about 950° C. to about 980° C. The source compounds in the first heating step can be heated at more than one temperature below about 850° C. In addition, the LiwCo1−xAxO2+y compound in the second heating step can be heated at more than one temperature from about 900° C. to about 1000° C. Preferably, the first heating step comprises heating the source compounds for a period of time of from about 30 minutes to about 3 hours and the second heating step comprises heating the source compounds for a period of time of from about 30 minutes to about 7 hours. The lithium source compound preferably used with the invention is selected from the group consisting of Li2CO3 and LiOH and the cobalt source compound is preferably selected from the group consisting of Co3O4 and Co(OH)2. The lithium cobalt oxide is preferably cooled after the heating steps at a rate of from 8° C./min to 140° C./min, more preferably from 10° C./min to 100° C./min.

[0014] The present invention further includes a method of analyzing a compound to determine if the compound is suitable for use as the active positive electrode material in a lithium or lithium-ion secondary battery. The method of the invention comprises determining a principal component space defined by the relationship axi+byi≦c, wherein xi={right arrow over (S)}i·{right arrow over (P)}c1; yi={right arrow over (S)}i·{right arrow over (P)}c2; the vector {right arrow over (S)}i is the x-ray spectrum for the compound; the vectors {right arrow over (P)}c1 and {right arrow over (P)}c2 are determined by measuring the x-ray powder diffraction values {right arrow over (S)}i for a predetermined range of 2θ values using a predetermined step size by sampling a plurality of samples of compounds having the same general formula as the compound and using the regression of {right arrow over (S)}i of the sample set against predetermined battery performance data for the samples by incorporating the samples as the positive electrode active material in a lithium or lithium-ion secondary battery. The xi and yi values for the compounds in the sample set that have the predetermined battery performance data are then used to determine a, b and c. The compound is analyzed by measuring the x-ray diffraction spectra for the compound to obtain x and y values and determining whether the x and y values meet the relationship axi+byi≦c and thus whether the compound possesses the battery performance and x-ray diffraction spectra suitable for use as the active positive electrode material.

[0015] The lithium cobalt oxides of the invention have good cycleability properties including good initial specific capacities and capacity fades and thus are desirable for use in rechargeable lithium and lithium-ion batteries. In addition, the lithium cobalt oxides of the present invention can be produced quickly in less than 10 hours and thus can be produced at a rate desired in the art.

[0016] These and other features and advantages of the present invention will become more readily apparent to those skilled in the art upon consideration of the following detailed description, which describes both the preferred and alternative embodiments of the present invention.

BRIEF DESCRIPTION OF THE DRAWINGS

[0017] FIG. 1 illustrates the positions of several samples in a principal component space as defined by the axes {right arrow over (P)}c1 and {right arrow over (P)}c2 with the dotted line representing x+0.77y=−6 in accordance with a preferred embodiment of the invention.

[0018] FIG. 2 illustrates the capacity fade after 50 cycles versus x+0.77y with the dotted line defining the principal component space of the samples of the invention having the desired x-ray powder diffraction values and a fade of less than or equal to 15% in accordance with a preferred embodiment of the invention.

DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS OF THE INVENTION

[0019] In the following detailed description, preferred embodiments are described in detail to enable practice of the invention. Although the invention is described with reference to these specific preferred embodiments, it will be understood that the invention is not limited to these preferred embodiments. But to the contrary, the invention includes numerous alternatives, modifications and equivalents as will become apparent from consideration of the following detailed description and accompanying drawings.

[0020] The present invention is directed to lithium cobalt oxides having the formula LiwCo1−xAxO2+y wherein 0.96≦w≦1.05, 0≦x≦0.05, −0.02≦y≦0.02 and A is one or more dopants. Preferably, 0.98≦w≦1.02 and 0≦x≦0.02. The dopants A are elements other than Co including metals and non-metals such as Ni, Mn, Ti, Zr, V, Mo, Mg, Ca, Sr, Ba, Al, Ga, Si, Ge, Sn, and combinations thereof. Preferably, the dopants A are selected to produce an oxidation state N wherein +2.5≦N≦+3.5, and preferably N is about 3. The average oxidation state N is based on the molar amounts of the dopants used and the valences of the dopants used. For example, if the dopants are 40% Ti4+ and 60% Mg2+, on a molar basis, the average oxidation state N would be (0.4)(+4)+(0.6)(+2)=+2.8.

[0021] The lithium cobalt oxides of the invention have a hexagonal layered crystal structure that is substantially single-phase and substantially free of localized cubic spinel-like structural phases on the surface of the crystal or within the crystal. The substantially single-phase, hexagonal layered structures of the compounds of the invention can be characterized, for example, by their powder x-ray diffraction patterns.

[0022] The lithium cobalt oxides of the present invention preferably have an initial specific discharge capacity of greater than or equal to 154 mAh/g and a capacity fade after 50 cycles of less than or equal to 15%. Specifically, when the lithium cobalt oxides are used as the positive electrode material in a lithium coin cell having a lithium negative electrode and the cell is cycled between 3.0 and 4.3V at a constant current of C/3 (3 hours for complete charge or discharge) during both the charge and discharge cycles, the cells have a capacity fade of less than or equal to 15% after 50 charge/discharge cycles. In these coin cells, NRC 2325 coin cell hardware and Celgard 3501 separators can be used. The electrolyte is typically 1M LiPF6 in a 50:50 mixture of ethylene carbonate and dimethyl carbonate solvents. In addition, the positive electrode consists generally of 85% active material (by weight), 10% super S™ carbon black and 5% polyvinylidene fluoride (PVDF) as a binder polymer, coated on aluminum foil.

[0023] The lithium cobalt oxides of the invention have a capacity fade of less than or equal to 15% after 50 cycles and can also be characterized by their x-ray powder diffraction patterns, which describe the crystal properties of the lithium cobalt oxides. In particular, the lithium cobalt oxides of the invention can be characterized by their positions in a principal component space determined by conducting principal component analysis of x-ray powder diffraction spectra between 15° and 120° using a 0.02° step size and CuKα rays. In the principal component analysis, each x-ray spectrum is treated as a vector {right arrow over (S)}i.

[0024] It has been discovered using this principal component analysis that the crystal properties that are important to the rechargeable lithium battery performance can be described in the space defined generally by two vectors, namely, principal components {right arrow over (P)}c1 and {right arrow over (P)}c2. These two vectors are preferably determined by using the partial least squares regression of {right arrow over (S)}i of a large sample set against the battery performance of the sample. This sample set includes lithium cobalt oxides having a capacity fade of less than or equal to 15% and lithium cobalt oxides having a capacity fade of greater than 15%.

[0025] The principal component space that includes the compounds of the invention having a capacity fade of less than or equal to 15% can be defined by the following relationship:

ax i +by i ≦c

[0026] wherein xi={right arrow over (S)}i·{right arrow over (P)}c1 (i.e. the projection of {right arrow over (S)}i onto {right arrow over (P)}c1); yi={right arrow over (S)}i·{right arrow over (P)}c2 (i.e. the projection of {right arrow over (S)}i onto {right arrow over (P)}c2); the vector {right arrow over (S)}i is the x-ray spectrum for the LiwCo1−xAxO2+y compound. The vectors {right arrow over (P)}c1 and {right arrow over (P)}c2 defining the principal component space can be determined by measuring the x-ray powder diffraction values {right arrow over (S)}i between 15° and 120° using a 0.02° step size and CuKα rays for a large sample set of lithium cobalt oxides and using the regression of {right arrow over (S)}iof the sample set against the capacity fade after 50 cycles of a lithium coin cell that includes a lithium negative electrode and the lithium cobalt oxide as the positive electrode material and that is cycled between 3.0 and 4.3V at a constant current of C/3 during both charge and discharge cycles. The values a, b and c of the above relationship can then be determined by using the xi and yi values for LiwCo1−xAxO2+y compounds in the sample set that have a capacity fade after 50 cycles of less than equal to 15%, i.e., the LiwCo1−xAxO2+y compounds prepared according to the invention.

[0027] The vector {right arrow over (S)}i is the x-ray diffraction spectrum of the ith sample and can be written as 1${\overrightarrow{S}}_i=\left(\begin{array}{c}⋮\\ s_{\mathrm{ij}}\\ ⋮\end{array}\right)$

[0028] where the element sij is the jth data point in the x-ray diffraction spectrum. In a partial least squares regression, the vector {right arrow over (S)}i is autoscaled before the regression takes place. The autoscaling of {right arrow over (S)}i is defined by 2${\overrightarrow{S}}_i^{\mathrm{as}}=\left(\begin{array}{c}⋮\\ s_{\mathrm{ij}}^{\mathrm{as}}\\ ⋮\end{array}\right)$

[0029] where the autoscaled element 3$s_{\mathrm{ij}}^{\mathrm{as}}=\frac{s_{\mathrm{ij}}-{\stackrel{\_}{s}}_j}{{\left(\frac{1}{n-1}\sum _i^n{\left(s_{\mathrm{ij}}-{\stackrel{\_}{s}}_j\right)}^2\right)}^{1/2}}$

[0030] and {overscore (s)}j is the mean of sij.

[0031] In the preferred embodiment of the invention, the regression is carried out with the commercial software Pirouette 2.7 available from Infometrix Inc., and the details of the matrix bidiagonalization algorithm is described in R. Marine, “Analysis of two partial least squares algorithms for multivariate calibration”, Chemom. Intell. Lab. Syst. 2, 187-197 (1987).

[0032] In accordance with a preferred embodiment of the invention, by using principal component analysis, the lithium cobalt oxides of the invention have a position within the principal component space defined by the following relationship:

x i +0.77yi≦−6

[0033] wherein xi={right arrow over (S)}i·{right arrow over (P)}c1; yi={right arrow over (S)}i·{right arrow over (P)}c2; {right arrow over (S)}i is the x-ray spectrum for the LiwCo1−xAxO2+y compound; and {right arrow over (P)}c1 and {right arrow over (P)}c2 are determined by measuring the x-ray powder diffraction values {right arrow over (S)}i between 15° and 120° using a 0.02° step size and CuKα rays for a large sample set of lithium cobalt oxides and using the partial least squares regression (PLSR) of {right arrow over (S)}i of the sample set against the capacity fade after 50 cycles of a lithium coin cell that includes a lithium negative electrode and the lithium cobalt oxide as the positive electrode material and that is cycled between 3.0 and 4.3V at a constant current of C/3 during both charge and discharge cycles. In particular, the vectors {right arrow over (P)}c1 and {right arrow over (P)}c2 can be defined by the coefficients provided in Table 1 below (wherein 2θ is the scattering angle for the x-ray powder diffraction measurements using CuKα rays). These measurements where obtained using a Rigaku RINT-2000 unit that includes a graphite monochrometer, a rotating anode x-ray source having a current of 150 mA and a voltage of 50 kV, anti-scattering slits set at 0.5°, and anti-divergence slits set at 0.5°. Alternative x-ray diffraction apparatus can also be used that produce comparable measurements to those produced with the above equipment and parameters.

	TABLE 1
	Coefficients of
	Principal
	Components
2θ (°)	Pc1	Pc2
15	−0.01379	0.011723
15.02	−0.02049	0.005086
15.04	0.006858	0.020376
15.06	−0.00273	0.013492
15.08	−0.01666	0.000753
15.1	0.000904	0.016155
15.12	−0.02289	0.001471
15.14	0.018222	0.020191
15.16	−0.00612	0.017684
15.18	−0.01378	0.008202
15.2	−0.0095	0.014128
15.22	−0.00584	0.010502
15.24	−0.00241	0.014185
15.26	−0.0042	0.014822
15.28	−0.00359	0.010447
15.3	−0.01418	0.009492
15.32	−0.01268	0.006936
15.34	−0.01096	0.001104
15.36	−0.00484	0.013178
15.38	−0.02337	−0.00186
15.4	−0.0185	0.005159
15.42	−0.01369	0.007337
15.44	−0.00748	0.015817
15.46	−0.00627	0.009999
15.48	0.002923	0.016611
15.5	−0.0327	−0.00277
15.52	−0.00977	0.009888
15.54	−0.01803	0.005404
15.56	−0.0272	−0.00066
15.58	−0.01839	0.006056
15.6	−0.0327	0.000501
15.62	0.001235	0.010506
15.64	0.004628	0.021154
15.66	−0.01218	0.011076
15.68	−0.01306	0.005821
15.7	0.017059	0.026611
15.72	−0.00215	0.017464
15.74	−0.0196	0.00594
15.76	−0.00819	0.015374
15.78	−0.00688	0.011794
15.8	0.01031	0.017391
15.82	−0.01997	−0.00295
15.84	−0.01823	0.006279
15.86	−0.00796	0.011133
15.88	−0.02731	0.001556
15.9	0.008318	0.01921
15.92	−0.0037	0.014344
15.94	0.007567	0.02072
15.96	−0.02027	0.003245
15.98	−0.01705	0.007303
16	−0.01747	0.00762
16.02	−0.0059	0.013742
16.04	−0.02571	0.000434
16.06	0.00123	0.015174
16.08	−0.02673	0.00081
16.1	0.000934	0.018006
16.12	0.017173	0.026867
16.14	−0.0108	0.007938
16.16	−0.00499	0.020462
16.18	−0.00362	0.016295
16.2	−0.00302	0.013994
16.22	−0.01649	0.005174
16.24	0.002657	0.011788
16.26	−0.01986	−0.0036
16.28	−0.01192	0.004226
16.3	−0.0216	0.002932
16.32	−0.03076	0.000359
16.34	−0.01702	0.005958
16.36	−0.02097	0.004851
16.38	−0.01344	0.012995
16.4	−0.01126	0.013165
16.42	0.001416	0.0201
16.44	0.025535	0.029834
16.46	−0.01265	0.005022
16.48	−0.01707	0.005082
16.5	0.005849	0.023367
16.52	0.003071	0.01825
16.54	−0.03934	−0.00869
16.56	−0.01295	0.008321
16.58	−0.00574	0.015581
16.6	−0.02828	−0.00285
16.62	−0.01588	0.006001
16.64	−0.01989	−0.00238
16.66	−0.02108	0.008733
16.68	−0.01442	0.008242
16.7	−0.00424	0.017365
16.72	−0.01095	0.007871
16.74	−0.00145	0.015669
16.76	−0.01792	0.005363
16.78	0.009292	0.023795
16.8	−0.00379	0.015671
16.82	−0.01185	0.007864
16.84	−0.01481	0.001576
16.86	−0.00946	0.009989
16.88	−0.00497	0.015388
16.9	−0.00746	0.01278
16.92	−0.03313	−0.00509
16.94	−0.01766	0.002109
16.96	−0.00494	0.01206
16.98	−0.00709	0.017855
17	−0.01431	0.006401
17.02	−0.01241	0.00343
17.04	−0.02585	−0.00416
17.06	−0.00734	0.00579
17.08	−0.03602	−0.00662
17.1	−0.00885	0.012849
17.12	−0.02162	0.003466
17.14	−0.01382	0.007276
17.16	0.002953	0.018335
17.18	0.006901	0.019663
17.2	−0.00352	0.020061
17.22	−0.02859	0.0027
17.24	−0.01144	0.012464
17.26	−0.03014	−0.00211
17.28	−0.0056	0.008632
17.3	−0.02932	0.000458
17.32	−0.01885	0.006068
17.34	−0.01338	0.009713
17.36	−0.01327	0.004136
17.38	−0.00626	0.012486
17.4	0.002288	0.017792
17.42	−0.00633	0.012048
17.44	−0.02932	−0.00294
17.46	−0.00039	0.014183
17.48	−0.01081	0.008801
17.5	−0.02267	−0.00304
17.52	0.003663	0.017713
17.54	−0.02049	0.000378
17.56	0.0067	0.021219
17.58	−0.01785	0.002949
17.6	0.001532	0.017236
17.62	−0.01238	0.007066
17.64	0.003693	0.012661
17.66	−0.01064	0.009715
17.68	−0.0185	0.00766
17.7	−0.00282	0.013796
17.72	−0.01224	0.007896
17.74	−0.03033	0.001698
17.76	−0.00672	0.014106
17.78	−0.00992	0.012609
17.8	−0.02352	−0.0001
17.82	−0.01922	0.004327
17.84	−0.03537	−0.00201
17.86	−0.00691	0.014539
17.88	−0.00823	0.010325
17.9	−0.01341	0.01078
17.92	0	0.013573
17.94	−0.01114	0.009463
17.96	−0.00572	0.008522
17.98	−0.02047	0.006135
18	−0.01031	0.010396
18.02	−0.00853	0.011528
18.04	−0.00317	0.013069
18.06	−0.01715	0.00713
18.08	−0.00062	0.020628
18.1	−0.00577	0.02002
18.12	−0.02559	0.008019
18.14	−0.01586	0.015835
18.16	0.000448	0.021869
18.18	−0.00187	0.022937
18.2	−0.00621	0.022318
18.22	−0.01021	0.016616
18.24	0.001908	0.025647
18.26	−0.00583	0.022761
18.28	0.00156	0.024646
18.3	−0.00703	0.021783
18.32	−0.00067	0.027247
18.34	−0.01602	0.016852
18.36	−0.01335	0.020628
18.38	−0.01909	0.01856
18.4	−0.02006	0.015536
18.42	−0.02351	0.014997
18.44	−0.02153	0.017015
18.46	−0.0188	0.017999
18.48	−0.01399	0.020999
18.5	−0.01053	0.02539
18.52	−0.00807	0.025661
18.54	−0.01182	0.02357
18.56	−0.01555	0.022593
18.58	−0.01783	0.020098
18.6	−0.01662	0.02401
18.62	−0.01523	0.024262
18.64	−0.01423	0.026318
18.66	−0.01205	0.026828
18.68	−0.00672	0.029541
18.7	−0.00607	0.028658
18.72	−0.00782	0.027355
18.74	−0.00921	0.026907
18.76	−0.01379	0.023838
18.78	−0.01457	0.023663
18.8	−0.01132	0.025623
18.82	−0.00952	0.026797
18.84	−0.00795	0.026828
18.86	−0.00768	0.02646
18.88	−0.01061	0.024087
18.9	−0.01522	0.015187
18.92	−0.01149	−0.00123
18.94	−0.003	−0.01538
18.96	0.004311	−0.01926
18.98	0.005713	−0.02314
19	0.005803	−0.02582
19.02	0.004528	−0.02683
19.04	0.001276	−0.02729
19.06	−0.00563	−0.02604
19.08	−0.01074	−0.02421
19.1	−0.01258	−0.02395
19.12	−0.01098	−0.02261
19.14	−0.00698	−0.01835
19.16	−0.00141	−0.01051
19.18	−0.00059	−0.00635
19.2	−0.00516	−0.00579
19.22	−0.01103	−0.00632
19.24	−0.01105	−0.0089
19.26	−0.00862	−0.0063
19.28	0.001626	0.001747
19.3	0.002138	0.004458
19.32	0.009506	0.005949
19.34	−0.02337	−0.00964
19.36	−0.00841	0.004954
19.38	−0.00834	−0.0036
19.4	−0.01069	0.001743
19.42	−0.01694	−0.00205
19.44	−0.00984	0.002493
19.46	0.001291	0.010088
19.48	−0.00713	0.004186
19.5	−0.01293	0.004569
19.52	−0.00902	0.005117
19.54	−0.02137	0.000343
19.56	−0.02552	0.000334
19.58	−0.00517	0.011511
19.6	−0.0205	0.00186
19.62	−0.0191	0.001679
19.64	−0.01089	0.005838
19.66	−0.0001	0.010501
19.68	−0.02876	−0.004
19.7	−0.01223	0.010851
19.72	−0.01543	0.005512
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19.98	−0.00695	0.013766
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20.36	−0.00825	0.012261
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20.98	0.005786	0.01745
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22.22	−0.00866	0.012586
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22.38	−0.0248	−0.00259
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22.98	−0.02426	−0.00322
23	−0.01972	0.000328
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23.64	−0.021	−0.00098
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24	−0.02221	0.004986
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24.06	−0.02615	−0.00314
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24.12	−0.03088	−0.00252
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24.16	−0.01106	0.003245
24.18	−0.02806	0.002902
24.2	−0.01107	0.010105
24.22	0.019514	0.023807
24.24	−0.00982	0.00959
24.26	−0.00739	0.006958
24.28	0.002216	0.01775
24.3	−0.017	0.003388
24.32	−0.01556	0.008514
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24.36	−0.00119	0.013486
24.38	−0.00266	0.015186
24.4	−0.02027	0.004786
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24.5	−0.01842	0.006243
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24.62	−0.0149	0.003534
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24.72	−0.02172	−0.00368
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24.86	−0.00677	0.012735
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24.96	−0.0031	0.010029
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25	−0.02494	−0.00192
25.02	−0.00857	0.010629
25.04	0.005546	0.016396
25.06	−0.00861	0.009162
25.08	−0.0262	0.000995
25.1	0.01366	0.023398
25.12	−0.0207	0.004447
25.14	−0.00097	0.014718
25.16	−0.02573	−0.00067
25.18	0.016504	0.027773
25.2	−0.00614	0.012067
25.22	−0.01746	0.009058
25.24	−0.03137	−0.00611
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25.28	−0.01941	−0.00035
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26	−0.0063	0.008874
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26.04	−0.00214	0.01381
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26.2	−0.00113	0.016394
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27	−0.00817	0.012676
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27.06	−0.02059	0.004236
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27.16	−0.00515	0.011742
27.18	−0.01706	0.008871
27.2	−0.01483	0.001105
27.22	0.000447	0.012124
27.24	−0.02892	−0.00354
27.26	−0.02499	−0.00131
27.28	−0.02738	0.000582
27.3	0.005241	0.016228
27.32	−0.00391	0.013754
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29.04	−0.02535	0.000098
29.06	−0.00397	0.013823
29.08	−0.01404	0.008431
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29.14	0.002258	0.018115
29.16	−0.01772	0.004794
29.18	0.001159	0.014385
29.2	−0.0092	0.007467
29.22	−0.01346	0.002319
29.24	−0.01994	0.006583
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29.4	0.020844	0.024903
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29.44	0.016068	0.028389
29.46	−0.00989	0.013432
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29.6	−0.00868	0.003539
29.62	−8.1E−05	0.009763
29.64	0.003099	0.018182
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29.7	−0.01604	0.002141
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29.76	−0.01385	0.001537
29.78	−0.02563	0.000812
29.8	0.013076	0.02172
29.82	−0.01258	0.007628
29.84	0.000264	0.014495
29.86	−0.00824	0.008593
29.88	−0.00551	0.014503
29.9	−0.00649	0.008497
29.92	−0.01026	0.009555
29.94	−0.00609	0.008309
29.96	0.008504	0.02317
29.98	−0.01651	−9.8E−05
30	−0.0032	0.016386
30.02	−0.00223	0.012625
30.04	−0.00942	0.00727
30.06	−0.01206	0.010086
30.08	−0.00652	0.009938
30.1	0.001475	0.01733
30.12	−0.00949	0.009564
30.14	0.001704	0.013136
30.16	−0.00656	0.009109
30.18	−0.02383	0.002381
30.2	0.002981	0.015583
30.22	−0.01309	0.005521
30.24	−0.00388	0.01764
30.26	0.00401	0.016784
30.28	−0.00331	0.011388
30.3	−0.01989	0.006512
30.32	0.001651	0.016746
30.34	0.004464	0.015515
30.36	−0.00731	0.016502
30.38	−0.00776	0.010328
30.4	0.023111	0.028897
30.42	−0.00235	0.018385
30.44	0.01111	0.021558
30.46	0.006027	0.026659
30.48	0.017769	0.023064
30.5	0.026135	0.033952
30.52	0.018123	0.025153
30.54	−0.00103	0.01352
30.56	0.013664	0.020386
30.58	0.011993	0.020279
30.6	0.002853	0.015146
30.62	0.024847	0.027579
30.64	−0.00832	0.008861
30.66	−0.0036	0.018022
30.68	0.032136	0.031088
30.7	0.013275	0.022551
30.72	−0.01891	0.002249
30.74	−0.01116	0.002116
30.76	−0.02445	0.004766
30.78	0.004683	0.018027
30.8	−0.02769	−0.00355
30.82	0.01378	0.021965
30.84	−0.02251	0.000829
30.86	−0.01897	0.000111
30.88	−0.00984	0.001934
30.9	0.001901	0.014832
30.92	−0.02704	−0.00171
30.94	0.014571	0.016324
30.96	−0.00113	0.010285
30.98	−0.00741	0.012472
31	−0.00665	0.013505
31.02	−0.01032	0.006826
31.04	−0.01092	0.00532
31.06	−0.00616	0.012151
31.08	−0.01764	0.004348
31.1	0.000624	0.017634
31.12	0.005639	0.023065
31.14	−0.01207	0.007302
31.16	0.000254	0.014257
31.18	−0.02295	−0.00033
31.2	−0.01528	0.002097
31.22	−0.00267	0.008824
31.24	−0.01234	0.008548
31.26	−0.01836	−0.00163
31.28	0.007313	0.021627
31.3	0.002849	0.016382
31.32	−0.00709	0.01347
31.34	−0.00308	0.011328
31.36	−0.01354	0.007043
31.38	−0.00502	0.010034
31.4	−0.03349	−0.00523
31.42	−0.01144	0.003559
31.44	−0.01968	−0.00161
31.46	−0.00152	0.013478
31.48	−0.00555	0.00926
31.5	0.030193	0.033035
31.52	−7.3E−05	0.01216
31.54	0.006864	0.017784
31.56	−0.01044	0.012269
31.58	0.030593	0.033164
31.6	−0.01115	0.009799
31.62	0.003676	0.016094
31.64	0.001955	0.015344
31.66	0.016509	0.028698
31.68	0.000465	0.017275
31.7	0.025884	0.03104
31.72	0.008125	0.019226
31.74	0.013191	0.023575
31.76	0.014479	0.02358
31.78	0.018473	0.029406
31.8	0.004989	0.016899
31.82	0.031748	0.031703
31.84	0.020072	0.028479
31.86	0.013073	0.02574
31.88	0.000985	0.015379
31.9	−0.01767	0.003861
31.92	0.01701	0.027537
31.94	0.019866	0.029487
31.96	−0.01266	0.005426
31.98	0.005567	0.02107
32	−0.01995	0.005691
32.02	−0.02459	−0.00245
32.04	−0.01932	0.003482
32.06	0.005429	0.020827
32.08	−0.01778	0.00395
32.1	−0.01029	0.005051
32.12	−0.00443	0.011386
32.14	0.003423	0.019453
32.16	−0.00569	0.013532
32.18	−0.00778	0.00714
32.2	−0.02025	0.001867
32.22	0.004379	0.017767
32.24	−0.02923	−0.00157
32.26	−0.01327	0.004046
32.28	−0.01906	0.002395
32.3	−0.00892	0.004087
32.32	0.005644	0.015182
32.34	−0.02007	0.004015
32.36	0.005043	0.015201
32.38	0.004733	0.019663
32.4	−0.01404	0.012699
32.42	0.032235	0.035912
32.44	−0.00028	0.015281
32.46	0.009437	0.02088
32.48	0.003368	0.018178
32.5	−0.01152	0.006845
32.52	−0.0292	0.00523
32.54	−0.00375	0.019224
32.56	−0.01017	0.009151
32.58	0.002898	0.011601
32.6	0.008722	0.019379
32.62	0.002746	0.011536
32.64	0.005034	0.015214
32.66	0.002667	0.020189
32.68	−0.00588	0.010532
32.7	−0.00463	0.0126
32.72	−0.0017	0.01345
32.74	−0.00694	0.007963
32.76	0.011784	0.019523
32.78	−0.00829	0.008339
32.8	0.003194	0.015366
32.82	−0.02057	0.004601
32.84	−0.02376	−0.00071
32.86	−0.00409	0.011251
32.88	−0.00469	0.014445
32.9	0.001594	0.017117
32.92	−0.01193	0.006187
32.94	−0.02586	0.003907
32.96	−0.01315	0.001155
32.98	−0.02658	−0.00299
33	0.006225	0.019847
33.02	−0.01973	0.006251
33.04	−0.02017	0.002713
33.06	0.01257	0.021751
33.08	−0.00871	0.010671
33.1	−0.01366	0.002939
33.12	−0.00459	0.010636
33.14	−0.00593	0.010916
33.16	0.001156	0.010902
33.18	−0.00892	0.003827
33.2	−0.00791	0.006356
33.22	−0.00919	0.013444
33.24	−0.02161	−3.7E−05
33.26	0.00199	0.013131
33.28	−0.00336	0.014706
33.3	−0.02591	0.000538
33.32	−0.00835	0.010279
33.34	0.006869	0.021395
33.36	−0.01945	0.002014
33.38	−0.01373	0.004159
33.4	−0.00412	0.006637
33.42	−0.01256	0.003792
33.44	0.004991	0.01703
33.46	−0.00026	0.012747
33.48	0.003139	0.015999
33.5	−0.00821	0.008497
33.52	−0.01395	0.007341
33.54	−0.01824	0.006169
33.56	−0.00705	0.01106
33.58	−0.00558	0.011178
33.6	0.002844	0.015366
33.62	−0.00182	0.016945
33.64	−0.01399	0.007736
33.66	0.006651	0.021143
33.68	−0.00741	0.009405
33.7	−0.01939	0.006642
33.72	−0.02219	−0.00053
33.74	0.00065	0.015869
33.76	0.013841	0.017178
33.78	0.011878	0.020543
33.8	−0.02161	−0.00179
33.82	−0.01516	0.006838
33.84	−0.0337	−0.00773
33.86	−0.00553	0.006652
33.88	−0.00346	0.010502
33.9	0.014919	0.02145
33.92	−0.00221	0.008853
33.94	0.017466	0.023787
33.96	−0.01672	0.001938
33.98	−0.03564	−0.00356
34	0.002283	0.016591
34.02	−0.00945	0.010918
34.04	−0.00947	0.011189
34.06	−0.00062	0.010941
34.08	−0.00222	0.013839
34.1	0.013336	0.020261
34.12	−0.00086	0.01424
34.14	−0.00297	0.013978
34.16	−0.004	0.011465
34.18	−0.0015	0.013011
34.2	0.016505	0.019066
34.22	−0.01874	−0.0022
34.24	−0.0228	−0.00229
34.26	−0.01549	0.004474
34.28	−0.02362	−0.00225
34.3	−0.01827	0.003237
34.32	0.008803	0.015433
34.34	−0.03694	−0.00986
34.36	−0.04722	−0.01675
34.38	−0.01057	0.005552
34.4	−0.01565	0.00636
34.42	−0.01861	0.000058
34.44	−0.01317	0.008012
34.46	0.004923	0.024582
34.48	0.007405	0.021616
34.5	−0.00471	0.015837
34.52	0.004011	0.009376
34.54	−0.00482	0.009305
34.56	0.01	0.015938
34.58	−0.01041	0.011472
34.6	−0.02353	0.000591
34.62	−0.01552	0.005716
34.64	−0.00242	0.009526
34.66	−0.00696	0.01039
34.68	0.002172	0.016381
34.7	−0.00084	0.01396
34.72	−0.0246	−0.00442
34.74	−0.01037	0.012368
34.76	−0.02537	0.006835
34.78	−0.00422	0.011447
34.8	0.011139	0.019368
34.82	−0.0106	0.006716
34.84	−0.04202	−0.00794
34.86	0.002865	0.016437
34.88	−0.03471	−0.01058
34.9	0.003278	0.014302
34.92	0.016522	0.019532
34.94	−0.00693	0.011526
34.96	−0.00439	0.007038
34.98	−0.00628	0.009208
35	−0.01262	0.005114
35.02	−0.01982	0.003502
35.04	0.005737	0.015192
35.06	−0.00214	0.018302
35.08	−0.00771	0.012526
35.1	0.009119	0.019586
35.12	−0.01811	0.001313
35.14	−0.0268	−0.00464
35.16	−0.00267	0.013068
35.18	−0.00951	0.004513
35.2	−0.02567	−0.00167
35.22	−0.02181	0.000775
35.24	−0.01087	0.007925
35.26	−0.01362	0.005992
35.28	−0.00517	0.011224
35.3	−0.00474	0.00729
35.32	−0.01081	0.008576
35.34	−0.01815	0.008631
35.36	0.009374	0.019001
35.38	−0.00678	0.008848
35.4	−0.03153	−0.00685
35.42	−0.02454	0.003717
35.44	0.007427	0.021312
35.46	0.020196	0.018474
35.48	−0.00155	0.007739
35.5	0.008345	0.020513
35.52	−0.00127	0.015958
35.54	−0.00113	0.009531
35.56	−0.01507	0.004768
35.58	0.010779	0.01968
35.6	−0.01315	0.006617
35.62	−0.00569	0.011114
35.64	−0.00159	0.018301
35.66	−0.00158	0.006585
35.68	−0.01076	0.010447
35.7	−0.02272	0.000283
35.72	−0.00648	0.010068
35.74	−0.01876	0.004051
35.76	−0.02052	0.004838
35.78	−0.01165	0.006354
35.8	−0.03664	−0.00645
35.82	−0.0062	0.016039
35.84	−0.0083	0.014194
35.86	−0.00858	0.005058
35.88	0.007249	0.019764
35.9	−0.0031	0.013031
35.92	−0.01974	0.002045
35.94	−0.01097	0.010728
35.96	−0.00183	0.008395
35.98	−0.00467	0.010105
36	0.004798	0.016298
36.02	−0.00114	0.008773
36.04	−0.01459	0.003437
36.06	0.016053	0.02293
36.08	0.01472	0.020758
36.1	−0.01364	0.007037
36.12	−0.02592	−0.00082
36.14	−0.00101	0.018409
36.16	0.001831	0.017042
36.18	−0.00765	0.005269
36.2	−0.00059	0.009734
36.22	−0.00929	0.008077
36.24	−0.02806	−0.001
36.26	−0.01306	0.008169
36.28	0.008648	0.019446
36.3	−0.01763	0.000977
36.32	0.01989	0.023905
36.34	−0.02686	0.000448
36.36	−0.00988	0.008583
36.38	−0.00441	0.010648
36.4	−0.00747	0.008667
36.42	−0.01358	0.003272
36.44	−0.00526	0.007282
36.46	0.008331	0.021593
36.48	0.006504	0.018276
36.5	−0.00687	0.009015
36.52	−0.00557	0.010854
36.54	−0.00313	0.008928
36.56	−0.00035	0.015287
36.58	−0.0152	−0.00251
36.6	−0.01613	0.008349
36.62	−0.00332	0.010132
36.64	−0.01691	0.005944
36.66	0.00509	0.015287
36.68	−0.00347	0.007346
36.7	0.002245	0.015181
36.72	−0.02243	−0.00367
36.74	−0.00027	0.00669
36.76	−0.01887	−0.00211
36.78	−0.00733	0.0075
36.8	−0.00839	0.00454
36.82	0.005324	0.007557
36.84	−0.00702	0.004762
36.86	0.013369	0.01396
36.88	−0.00469	−0.00057
36.9	−0.01001	−0.00115
36.92	0.008325	0.010895
36.94	−0.0079	0.006352
36.96	−0.00982	0.005495
36.98	−0.00329	0.008544
37	−0.01053	0.010457
37.02	−0.00882	0.015864
37.04	0.009285	0.027611
37.06	−0.00413	0.022436
37.08	−0.00846	0.019435
37.1	−0.00522	0.024844
37.12	−0.01819	0.018777
37.14	−0.013	0.025585
37.16	−0.00916	0.027147
37.18	−0.00965	0.027117
37.2	−0.01576	0.023712
37.22	−0.01588	0.024411
37.24	−0.02041	0.021323
37.26	−0.01909	0.022525
37.28	−0.01657	0.023997
37.3	−0.0175	0.023549
37.32	−0.01702	0.02322
37.34	−0.01774	0.023137
37.36	−0.02396	0.019223
37.38	−0.02314	0.012443
37.4	−0.00635	−0.00316
37.42	0.013541	−0.01083
37.44	0.015086	−0.01257
37.46	−0.0007	−0.01329
37.48	−0.01609	−0.01843
37.5	−0.00035	−0.02139
37.52	0.015298	−0.01877
37.54	0.015279	−0.02063
37.56	0.013541	−0.01996
37.58	0.003797	−0.02092
37.6	−0.00519	−0.02077
37.62	−0.00597	−0.01952
37.64	−0.00931	−0.02033
37.66	−0.00143	−0.01362
37.68	−0.00278	−0.0039
37.7	−0.01224	−0.00584
37.72	−0.00687	−0.00473
37.74	−0.00621	0.001787
37.76	0.007666	0.005383
37.78	−0.01494	0.00047
37.8	−0.01318	0.000854
37.82	0.005312	0.022019
37.84	−0.00329	0.017552
37.86	−0.01262	0.004109
37.88	−0.00918	0.010258
37.9	−0.02066	0.000259
37.92	−0.02209	0.000991
37.94	−0.01143	0.008404
37.96	−0.0028	0.013546
37.98	−0.00455	0.010294
38	−0.00196	0.015279
38.02	−0.00038	0.018473
38.04	0.005849	0.019527
38.06	−0.00101	0.018423
38.08	0.004052	0.02103
38.1	−0.01651	0.012178
38.12	−0.005	0.025003
38.14	−0.01566	0.015165
38.16	0.00228	0.030547
38.18	−0.0104	0.020912
38.2	−0.00987	0.024819
38.22	−0.00295	0.028311
38.24	−0.00817	0.025126
38.26	0.000071	0.030764
38.28	−0.01174	0.024131
38.3	−0.01014	0.026126
38.32	−0.01341	0.024132
38.34	−0.01344	0.023197
38.36	−0.01476	0.01989
38.38	−0.01401	0.009605
38.4	0.003812	−0.0008
38.42	0.012143	−0.01294
38.44	0.015499	−0.01359
38.46	0.009391	−0.01748
38.48	−0.00321	−0.02057
38.5	0.004162	−0.01609
38.52	0.01066	−0.01951
38.54	0.014858	−0.01975
38.56	0.016969	−0.01951
38.58	0.012016	−0.02129
38.6	−0.00584	−0.02651
38.62	−0.007	−0.01784
38.64	−0.00046	−0.00909
38.66	0.005252	0.007621
38.68	0.007242	0.015764
38.7	0.008513	0.016245
38.72	0.007346	0.021039
38.74	−0.02044	0.005124
38.76	−0.00054	0.020978
38.78	−0.00949	0.019303
38.8	−0.03259	0.004364
38.82	−0.01554	0.017219
38.84	−0.02864	0.014419
38.86	−0.0127	0.022256
38.88	−0.00528	0.029242
38.9	−0.01632	0.020757
38.92	−0.01133	0.02495
38.94	−0.01291	0.025584
38.96	−0.0185	0.022869
38.98	−0.0134	0.025426
39	−0.01134	0.026429
39.02	−0.01531	0.024395
39.04	−0.01442	0.022007
39.06	−0.01211	0.004554
39.08	0.009892	−0.01012
39.1	0.020535	−0.01101
39.12	0.011887	−0.01293
39.14	−0.0138	−0.01464
39.16	−0.01067	−0.01762
39.18	0.00412	−0.02285
39.2	0.017982	−0.01844
39.22	0.013978	−0.02114
39.24	0.009008	−0.02217
39.26	−0.00018	−0.02046
39.28	−0.00504	−0.01666
39.3	−0.00396	−0.0139
39.32	0.003972	−0.00169
39.34	−0.01121	−0.01286
39.36	−0.00271	0.004501
39.38	0.019857	0.025798
39.4	−0.01694	−0.00112
39.42	−0.00456	0.009305
39.44	−0.01411	0.003253
39.46	0.02052	0.024105
39.48	0.002086	0.012012
39.5	−0.01084	0.009234
39.52	0.009228	0.017061
39.54	−0.00665	0.009525
39.56	0.012552	0.01857
39.58	0.00452	0.014193
39.6	0.00228	0.012717
39.62	−0.00301	0.01298
39.64	−0.00693	0.007842
39.66	0.014476	0.023379
39.68	−0.00225	0.012816
39.7	−0.0182	0.005316
39.72	−0.02555	0.002669
39.74	−0.00967	0.010916
39.76	−0.00369	0.018493
39.78	−0.01853	0.00174
39.8	0.018086	0.025473
39.82	−0.01644	0.009201
39.84	0.035291	0.03467
39.86	0.001612	0.014123
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53.36	−0.00966	0.006573
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53.54	−0.01172	0.005681
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54.2	−0.01079	0.00392
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55.18	−0.03482	−0.00642
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55.22	0.024286	0.022673
55.24	−0.00744	0.014658
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55.28	−0.02021	0.002805
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55.38	0.007585	0.013766
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55.5	−0.0026	0.011792
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56.16	−0.00577	0.012792
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56.24	−0.01994	−0.00064
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56.4	−0.02037	−0.00018
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57.34	−0.02996	−0.00786
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58.22	−0.00347	0.015892
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62.3	−0.00086	0.012238
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62.78	−0.02453	−0.0012
62.8	0.004087	0.017609
62.82	0.002593	0.012223
62.84	0.006462	0.025534
62.86	0.019587	0.025675
62.88	−0.00428	0.004919
62.9	−0.00689	0.003587
62.92	0.020156	0.023848
62.94	−0.01012	0.010305
62.96	−0.01883	−0.00443
62.98	0.006674	0.015884
63	−0.02079	0.006183
63.02	−0.0128	0.003578
63.04	−0.00031	0.015328
63.06	−0.01922	0.004119
63.08	−0.00204	0.013878
63.1	0.000992	0.014996
63.12	0.030637	0.029326
63.14	−0.00061	0.015297
63.16	−0.00379	0.015885
63.18	−0.00725	0.005162
63.2	−0.01624	0.006375
63.22	−0.00103	0.018569
63.24	0.005798	0.020726
63.26	0.003658	0.015261
63.28	0.003847	0.017328
63.3	−0.021	−0.00373
63.32	0.003128	0.015608
63.34	−0.00148	0.012731
63.36	−0.01122	0.007242
63.38	−0.00654	0.008314
63.4	−0.00461	0.01125
63.42	0.000193	0.01638
63.44	−0.01314	0.002084
63.46	−0.01282	0.012267
63.48	0.015168	0.027305
63.5	−0.02366	0.003161
63.52	−0.01414	0.006139
63.54	−0.01012	0.00575
63.56	−0.0136	0.006203
63.58	0.000007	0.010688
63.6	0.019995	0.027301
63.62	−0.00451	0.013964
63.64	−0.00956	0.010486
63.66	−0.02425	0.001904
63.68	−0.01339	0.005909
63.7	−0.01386	0.001977
63.72	0.011416	0.026609
63.74	−0.00844	0.007653
63.76	−0.00468	0.008722
63.78	−0.01396	0.006371
63.8	0.006471	0.016748
63.82	−0.01453	−0.00153
63.84	0.015301	0.021849
63.86	−0.01951	0.001212
63.88	−0.00407	0.012369
63.9	0.006023	0.016845
63.92	−0.00345	0.009416
63.94	0.007054	0.020912
63.96	−0.0082	0.003415
63.98	−0.02431	−0.00364
64	−0.01781	0.00536
64.02	−0.03023	−0.00701
64.04	−0.01368	0.005304
64.06	−0.00459	0.014432
64.08	0.0039	0.018818
64.1	−0.00216	0.012226
64.12	−0.00216	0.014183
64.14	−0.01336	0.009749
64.16	−0.03045	−0.01094
64.18	−0.01973	0.003458
64.2	−0.01586	0.005682
64.22	−0.00346	0.01247
64.24	−0.00476	0.010972
64.26	0.015917	0.022256
64.28	0.002906	0.015343
64.3	0.005067	0.017523
64.32	0.003986	0.019308
64.34	−0.02232	−0.00407
64.36	−0.01404	0.007916
64.38	0.001525	0.015904
64.4	−0.00626	0.003569
64.42	−1.2E−05	0.012571
64.44	0.000781	0.008328
64.46	0.016502	0.023736
64.48	−0.00977	0.005516
64.5	0.010132	0.022211
64.52	−0.0164	0.002803
64.54	0.012748	0.027626
64.56	−0.0074	0.01236
64.58	−0.00231	0.016093
64.6	0.021028	0.031251
64.62	−0.03053	−0.01124
64.64	−0.01197	0.004527
64.66	−0.02668	−0.00636
89.52	0.006655	0.015242
89.54	−0.0019	0.010947
89.56	−0.02067	0.001522
89.58	−0.01371	0.00795
89.6	−0.03057	−0.0022
89.62	0.01032	0.018621
89.64	−0.02588	0.000776
89.66	−0.00164	0.013302
89.68	0.005274	0.02168
89.7	−0.00254	0.009249
89.72	−0.01147	0.010923
89.74	0.012789	0.022655
89.76	0.014879	0.017936
89.78	−0.0072	0.009961
89.8	0.00814	0.02357
89.82	−0.00707	0.006861
89.84	−0.00661	0.012538
89.86	0.001584	0.017567
89.88	−0.00699	0.011558
89.9	−0.01167	0.006483
89.92	0.023649	0.026408
89.94	−0.01065	0.003718
89.96	−0.00437	0.011189
89.98	−0.00617	0.007667
90	−0.02426	−0.00405
90.02	−7E−06	0.010775
90.04	−0.01148	0.006576
90.06	0.005918	0.014726
90.08	−0.00431	0.00769
90.1	−0.02011	−0.00036
90.12	−0.00448	0.011677
90.14	−0.0104	0.005563
90.16	0.020222	0.023218
90.18	−0.00443	0.00521
90.2	0.011742	0.019435
90.22	−0.00238	0.016925
90.24	−0.00433	0.015195
90.26	−0.00734	0.0131
90.28	−0.02347	−0.00121
90.3	−0.0017	0.010209
90.32	−0.00446	0.006142
90.34	−0.01142	0.011989
90.36	0.002501	0.017676
90.38	−0.02856	−0.00186
90.4	−0.00632	0.007122
90.42	−0.00759	0.007806
90.44	−0.00036	0.013945
90.46	−0.03349	−0.00595
90.48	−0.00656	0.011259
90.5	−0.02447	−0.00076
90.52	0.010318	0.020981
90.54	−0.01001	0.010745
90.56	0.010035	0.025269
90.58	0.007286	0.015892
90.6	−0.00807	0.009989
90.62	0.008209	0.018393
90.64	−0.00978	0.004064
90.66	−0.00567	0.015367
90.68	−0.00814	0.013789
90.7	−0.00991	0.009934
90.72	−0.01475	0.001774
90.74	−0.01172	0.016758
90.76	−0.00877	0.006296
90.78	0.007077	0.021212
90.8	−0.00283	0.010971
90.82	−0.00243	0.015305
90.84	0.00041	0.019241
90.86	0.004265	0.016742
90.88	−0.00747	0.007768
90.9	−0.00321	0.013472
90.92	0.016085	0.027818
90.94	−0.02508	−0.00086
90.96	−0.00377	0.013107
90.98	−0.0208	0.005208
91	0.037425	0.035216
91.02	−0.00155	0.012794
91.04	−0.00261	0.013818
91.06	0.001771	0.013968
91.08	−0.0096	0.005273
91.1	−0.00865	0.008971
91.12	0.004783	0.017934
91.14	−0.00908	0.01095
91.16	0.014322	0.023846
91.18	−0.00733	0.008356
91.2	0.018566	0.028553
91.22	−0.00252	0.014053
91.24	−0.00188	0.016565
91.26	0.004981	0.017588
91.28	−0.00501	0.009944
91.3	−0.01001	0.008749
91.32	−0.00037	0.017141
91.34	−0.01181	0.005604
91.36	−0.0218	−0.00031
91.38	−0.0119	0.005317
91.4	0.005446	0.02133
91.42	−0.01182	0.007892
91.44	−0.016	0.005633
91.46	−0.00144	0.016674
91.48	−0.00834	0.00876
91.5	0.001963	0.011171
91.52	−0.01012	0.013185
91.54	0.016591	0.025673
91.56	−0.00033	0.018007
91.58	0.008808	0.018747
91.6	−0.00108	0.017486
91.62	−0.00371	0.018634
91.64	−0.00855	0.01203
91.66	−0.00836	0.005923
91.68	−0.0106	0.005394
91.7	−0.0023	0.01442
91.72	0.002803	0.016435
91.74	−0.00626	0.013165
91.76	−0.01155	0.009757
91.78	−0.01391	0.007977
91.8	0.000091	0.013402
91.82	−0.00504	0.015388
91.84	−0.01583	0.003168
91.86	0.005365	0.014744
91.88	−0.02528	−0.00497
91.9	0.006403	0.016455
91.92	−0.01059	0.008905
91.94	−0.01645	0.005791
91.96	−0.00824	0.014027
91.98	0.007091	0.022271
92	−0.0056	0.009453
92.02	0.002611	0.00924
92.04	−0.00458	0.016519
92.06	−0.01167	0.005253
92.08	0.002284	0.008293
92.1	−0.03021	−0.00493
92.12	0.002725	0.013863
92.14	−0.01464	0.002114
92.16	−0.02234	−0.00236
92.18	−0.00393	0.007137
92.2	−0.00976	0.005943
92.22	−0.00158	0.010607
92.24	−0.01497	0.007923
92.26	0.003957	0.013401
92.28	−0.00878	0.005291
92.3	−0.00649	0.012994
92.32	−0.02434	−0.00506
92.34	−0.00655	0.006006
92.36	−0.00718	0.012062
92.38	−0.01509	0.0045
92.4	0.009706	0.017495
92.42	0.014932	0.024001
92.44	0.001383	0.011733
92.46	−0.00754	0.00814
92.48	0.03364	0.026474
92.5	−0.00431	0.010538
92.52	0.004286	0.01299
92.54	−0.00799	0.009992
92.56	0.012932	0.022878
92.58	−0.0148	0.004956
92.6	−0.01048	0.006947
92.62	−0.0194	−0.00283
92.64	−0.00408	0.010232
92.66	−0.01524	0.00535
92.68	0.002246	0.013341
92.7	0.0038	0.019411
92.72	−0.00469	0.014537
92.74	0.016175	0.016743
92.76	0.005706	0.019522
92.78	0.00874	0.019941
92.8	−0.0342	−0.0099
92.82	0.006438	0.013341
92.84	0.013342	0.02232
92.86	−0.00665	0.013501
92.88	−0.01185	0.010405
92.9	0.001541	0.012047
92.92	−0.01275	0.006972
92.94	0.010173	0.015722
92.96	−0.01044	0.00751
92.98	−0.01159	0.013476
93	−0.00977	0.003812
93.02	−0.02728	0.000927
93.04	0.017043	0.02111
93.06	−0.01648	0.002594
93.08	−0.02611	−0.00059
93.1	−0.01872	0.004065
93.12	0.009653	0.021291
93.14	−0.00602	0.012844
93.16	−0.0093	0.014221
93.18	0.009397	0.02152
93.2	−0.02351	0.003003
93.22	−0.01243	0.005577
93.24	0.001363	0.013466
93.26	−0.01968	−0.00299
93.28	−0.03013	−0.0023
93.3	0.002845	0.011472
93.32	0.018995	0.020201
93.34	0.010549	0.022875
93.36	0.004251	0.014681
93.38	−0.01883	−0.00528
93.4	0.001557	0.011899
93.42	0.020871	0.026288
93.44	−0.00405	0.010946
93.46	−0.00819	0.012089
93.48	−0.00903	0.010638
93.5	−0.00957	0.010535
93.52	0.003931	0.015278
93.54	−0.00958	0.010639
93.56	−0.01013	0.010695
93.58	−0.00406	0.015074
93.6	0.001499	0.01712
93.62	−0.01132	0.002472
93.64	−0.03153	−0.00171
93.66	−0.03303	−0.01212
93.68	0.000159	0.016635
93.7	−0.00087	0.013649
93.72	−0.00334	0.011179
93.74	−0.0135	0.00358
93.76	−0.00653	0.012206
93.78	−0.01347	0.001919
93.8	−0.02147	0.002208
93.82	0.000788	0.014145
93.84	0.009397	0.017396
93.86	−0.00201	0.009651
93.88	0.002365	0.016807
93.9	0.011285	0.01862
93.92	0.000441	0.01608
93.94	−0.01294	0.005954
93.96	−8.7E−05	0.011549
93.98	−0.01413	0.007593
94	−0.00143	0.01382
94.02	−0.00066	0.013175
94.04	0.00817	0.021327
94.06	−0.01758	0.005248
94.08	−0.0027	0.008285
94.1	−0.00602	0.011342
94.12	−0.00514	0.010048
94.14	−0.00397	0.006079
94.16	0.008634	0.019766
94.18	0.003734	0.0138
94.2	−0.01603	0.000736
94.22	−0.00472	0.011402
94.24	−0.00878	0.013639
94.26	−0.01888	0.001362
94.28	0.003616	0.01581
94.3	−0.01929	−0.0001
94.32	0.014444	0.014736
94.34	0.003362	0.021684
94.36	0.01309	0.018782
94.38	−0.01333	0.007945
94.4	0.009827	0.016593
94.42	0.000857	0.017108
94.44	−0.0064	0.00536
94.46	−0.00486	0.009009
94.48	−0.00751	0.010624
94.5	−0.01899	0.002567
94.52	0.019313	0.034425
94.54	0.008119	0.021532
94.56	−0.03181	−0.00192
94.58	−0.02795	0.000512
94.6	−0.00403	0.014726
94.62	0.012935	0.028182
94.64	−0.00588	0.012211
94.66	−0.00043	0.020238
94.68	−0.01189	0.012787
94.7	−0.0147	0.013795
94.72	−0.02648	0.008367
94.74	−0.01899	0.015768
94.76	−0.01859	0.017224
94.78	−0.01831	0.019365
94.8	−0.032	0.00861
94.82	−0.01597	0.020651
94.84	−0.0217	0.01289
94.86	−0.03039	−0.0007
94.88	−0.0076	0.005931
94.9	0.017245	−0.00113
94.92	0.026285	−0.00905
94.94	0.0145	−0.01988
94.96	0.0222	−0.01453
94.98	0.01716	−0.01174
95	−0.00508	−0.01172
95.02	0.002951	0.002351
95.04	−0.01787	−0.00522
95.06	−0.01439	0.00858
95.08	−0.01065	0.012479
95.1	−0.00713	0.021446
95.12	−0.02316	0.013925
95.14	−0.02625	0.015742
95.16	−0.02713	0.014925
95.18	−0.03333	0.006785
95.2	−0.0137	0.017007
95.22	−0.00692	0.011962
95.24	−0.01582	0.008026
95.26	−0.0235	0.001787
95.28	−0.01053	0.00372
95.3	0.00483	−4.5E−05
95.32	0.010134	−0.00925
95.34	0.020663	−0.01364
95.36	0.022731	−0.01354
95.38	0.011812	−0.01582
95.4	−0.00262	−0.01596
95.42	−0.00153	−0.01031
95.44	−0.00295	−0.00737
95.46	−0.00725	0.005015
95.48	−0.00732	0.005041
95.5	−0.02051	0.00303
95.52	−0.02776	0.007259
95.54	−0.01598	0.017559
95.56	−0.02931	0.011751
95.58	−0.0169	0.017071
95.6	−0.01135	0.013272
95.62	0.008339	0.011926
95.64	0.014559	−0.00544
95.66	0.010931	−0.01359
95.68	0.025076	−0.00446
95.7	0.010887	−0.00705
95.72	0.000276	−0.00981
95.74	−0.00591	−0.00504
95.76	−0.01359	−0.00745
95.78	−0.00375	0.004032
95.8	0.020589	0.021199
95.82	0.001056	0.009056
95.84	−0.01457	−0.00118
95.86	−0.01092	0.002145
95.88	0.041194	0.029969
95.9	−0.00246	0.012876
95.92	0.023196	0.029119
95.94	−0.00226	0.014568
95.96	−0.01742	0.002935
95.98	−0.00261	0.016495
96	0.010967	0.02195
96.02	−0.01425	0.004313
96.04	0.003763	0.017739
96.06	−0.00756	0.007731
96.08	0.004358	0.01798
96.1	−0.03493	−0.00621
96.12	0.01099	0.017964
96.14	0.004917	0.016056
96.16	−0.00975	0.008076
96.18	−0.01499	0.00945
96.2	−0.00982	0.009573
96.22	−0.0023	0.013396
96.24	0.005115	0.021117
96.26	−0.01047	0.008427
96.28	−0.0097	0.002165
96.3	−0.0105	0.005453
96.32	−0.02268	0.001266
96.34	−0.01802	0.005726
96.36	0.000488	0.015398
96.38	0.014841	0.021034
96.4	−0.03167	−0.00713
96.42	−0.01662	−0.00119
96.44	−0.00136	0.01427
96.46	−0.00838	0.012509
96.48	−0.02336	−0.00082
96.5	0.022216	0.027028
96.52	−0.00397	0.013703
96.54	−0.00997	0.005578
96.56	−0.00457	0.010438
96.58	0.018634	0.021874
96.6	0.03265	0.034483
96.62	0.002709	0.01983
96.64	−0.02497	−0.00287
96.66	−0.01527	0.000748
96.68	−0.00809	0.011409
96.7	−0.01255	0.010797
96.72	−8.8E−05	0.018356
96.74	0.002456	0.007942
96.76	0.018321	0.024654
96.78	−0.00737	0.003998
96.8	0.011062	0.01954
96.82	−0.00984	0.014959
96.84	−0.00144	0.01588
96.86	0.006184	0.018104
96.88	0.006517	0.016941
96.9	−0.02209	0.006125
96.92	−0.00848	0.006556
96.94	0.009841	0.028004
96.96	0.010933	0.017222
96.98	−0.0009	0.016624
97	−0.01845	0.004593
97.02	−0.02132	−0.0041
97.04	−0.00024	0.014172
97.06	−0.00608	0.006352
97.08	−0.00465	0.011451
97.1	0.020227	0.024024
97.12	0.008369	0.0187
97.14	−0.02794	−0.00043
97.16	−0.0202	−0.00154
97.18	0.022306	0.028938
97.2	−0.00398	0.009137
97.22	−0.00222	0.011986
97.24	−0.00632	0.00794
97.26	0.014781	0.024531
97.28	−0.01371	0.00717
97.3	0.000306	0.015452
97.32	0.002514	0.016285
97.34	−0.00643	0.013339
97.36	0.008754	0.015845
97.38	−0.01948	0.002572
97.4	−0.00784	0.004465
97.42	0.026494	0.030718
97.44	0.020896	0.030357
97.46	0.002699	0.015392
97.48	−0.0204	0.003685
97.5	0.004597	0.010975
97.52	−0.00133	0.013252
97.54	−0.02556	−0.00515
97.56	0.005127	0.017028
97.58	−0.02744	−0.00038
97.6	−0.01024	0.005713
97.62	−0.00321	0.012341
97.64	0.002554	0.019916
97.66	0.00091	0.013798
97.68	−0.01281	0.007732
97.7	−0.02171	0.00281
97.72	−0.00531	0.015187
97.74	0.022015	0.020397
97.76	−0.03186	−0.00105
97.78	0.001821	0.018245
97.8	0.008969	0.021012
97.82	−0.00593	0.010264
97.84	0.000766	0.015041
97.86	−0.01006	0.005704
97.88	−0.01707	−0.0002
97.9	−0.00737	0.001703
97.92	−0.01126	0.011801
97.94	0.011739	0.021738
97.96	0.02248	0.024454
97.98	−0.00437	0.014903
98	−0.02344	−0.00077
98.02	−0.0236	0.001717
98.04	0.002901	0.013718
98.06	−0.01196	0.00793
98.08	0.004469	0.017296
98.1	−0.01177	0.0069
98.12	0.000196	0.01108
98.14	−0.02324	0.001754
98.16	−0.00746	0.013496
98.18	−0.00919	0.005154
98.2	−0.03344	−0.00703
98.22	−0.00339	0.009853
98.24	−0.02052	−0.0021
98.26	−0.03006	−0.00746
98.28	0.00164	0.012673
98.3	0.014273	0.020776
98.32	0.006998	0.016568
98.34	0.003262	0.017708
98.36	−0.00383	0.013683
98.38	0.002925	0.017607
98.4	−0.00118	0.016687
98.42	−0.00222	0.013767
98.44	−0.02168	0.006042
98.46	−0.00231	0.021138
98.48	−0.00923	0.008992
98.5	0.000614	0.011492
98.52	0.010107	0.026301
98.54	0.00421	0.016297
98.56	−0.01181	0.005763
98.58	−0.00916	0.010457
98.6	0.015388	0.022566
98.62	−0.00934	0.008565
98.64	0.001192	0.01252
98.66	0.000053	0.015886
98.68	−0.02442	−0.00271
98.7	−0.03062	−0.00825
98.72	0.007347	0.022286
98.74	−0.00738	0.010671
98.76	−0.00501	0.01438
98.78	0.012455	0.022171
98.8	−0.0312	−0.00595
98.82	−0.01639	0.008919
98.84	−0.01257	0.007097
98.86	−0.00595	0.008072
98.88	−0.00597	0.008454
98.9	0.007109	0.01434
98.92	0.00929	0.016896
98.94	0.007131	0.015473
98.96	0.011004	0.015958
98.98	−0.01444	0.004022
99	0.010033	0.02323
99.02	0.004684	0.019776
99.04	−0.01486	0.004631
99.06	−0.00768	0.00999
99.08	−0.02031	0.009953
99.1	−0.00162	0.010631
99.12	−0.0386	−0.00557
99.14	−0.01507	0.005062
99.16	−0.00175	0.012583
99.18	−0.02435	−0.00527
99.2	−0.00527	0.009045
99.22	0.007757	0.015674
99.24	0.006267	0.020987
99.26	−0.00152	0.007254
99.28	−0.00143	0.010325
99.3	0.000817	0.018159
99.32	−0.01391	0.004613
99.34	0.003704	0.015594
99.36	0.01366	0.020613
99.38	0.029762	0.030156
99.4	0.008411	0.020473
99.42	−0.00893	0.008739
99.44	−0.00248	0.007544
99.46	−0.01309	0.004822
99.48	0.014431	0.020727
99.5	−0.00117	0.01058
99.52	−0.03031	0.00101
99.54	−0.00732	0.010904
99.56	−0.01143	0.002656
99.58	0.006772	0.018867
99.6	0.010089	0.023518
99.62	−0.01458	0.011218
99.64	0.006115	0.014539
99.66	−0.01602	0.007622
99.68	0.010039	0.017619
99.7	−0.00936	0.012649
99.72	−0.00741	0.006961
99.74	−0.01896	0.006195
99.76	0.00114	0.013893
99.78	−0.00037	0.01289
99.8	0.005217	0.015818
99.82	−0.00179	0.015437
99.84	−0.02013	−0.00224
99.86	−0.00088	0.016458
99.88	−0.00454	0.009234
99.9	−0.02808	−0.00418
99.92	−0.01925	0.001305
99.94	0.010311	0.017051
99.96	0.007433	0.022128
99.98	−0.01056	0.01018
100	−0.01744	−0.00014
100.02	−0.00825	0.00988
100.04	−0.01019	0.005338
100.06	−0.00381	0.010007
100.08	−0.02345	−0.0068
100.1	−0.00909	0.001209
100.12	0.006211	0.017113
100.14	0.004318	0.023212
100.16	−0.00193	0.021418
100.18	−0.01934	0.005104
100.2	−0.00788	0.013122
100.22	−0.01541	0.002889
100.24	−0.01637	0.011143
100.26	−0.01762	0.011124
100.28	−0.00891	0.018841
100.3	−0.01413	0.01281
100.32	−0.01579	0.01492
100.34	−0.02201	0.014733
100.36	−0.02077	0.014601
100.38	−0.01568	0.01562
100.4	−0.03081	0.012078
100.42	−0.02337	0.016766
100.44	−0.02411	0.015681
100.46	−0.03084	0.008382
100.48	−0.02927	0.006706
100.5	−0.01335	0.004202
100.52	−0.01337	−0.01113
100.54	0.00845	−0.011
100.56	0.020217	−0.01445
100.58	0.021811	−0.01344
100.6	0.009572	−0.01855
100.62	0.00829	−0.01411
100.64	0.004338	−0.00956
100.66	0.006413	0.006565
100.68	−0.00806	−0.00156
100.7	−0.01107	−5.4E−05
100.72	−0.01101	0.005605
100.74	−0.00956	0.017976
100.76	−0.02108	0.012889
100.78	−0.01394	0.021431
100.8	−0.0345	0.00599
100.82	−0.02887	0.008155
100.84	−0.0225	0.00445
100.86	0.003469	0.006826
100.88	−0.00075	−0.0099
100.9	0.016538	−0.00915
100.92	0.013925	−0.01513
100.94	0.0208	−0.01078
100.96	0.006313	−0.0148
100.98	0.022736	0.002303
101	0.018185	0.009012
101.02	−0.00369	−0.0035
101.04	−0.00557	0.003374
101.06	0.002134	0.003779
101.08	0.013142	0.011529
101.1	−0.00095	0.005538
101.12	−0.01496	−0.00043
101.14	−0.02177	−0.00263
101.16	0.010296	0.016799
101.18	−0.02214	−0.00823
101.2	−0.00109	0.013985
101.22	−0.01383	0.004048
101.24	−0.00574	0.012326
101.26	−0.01744	0.004786
101.28	−0.00199	0.012136
101.3	−0.02616	−0.00055
101.32	−0.00112	0.014359
101.34	−0.00844	0.007451
101.36	−0.00182	0.006139
101.38	0.007273	0.01573
101.4	0.00279	0.009523
101.42	0.01701	0.025821
101.44	−0.00091	0.015598
101.46	0.0084	0.021568
101.48	0.009606	0.020732
101.5	−0.01853	0.001749
101.52	0.00385	0.0194
101.54	−0.0189	0.002082
101.56	−0.01289	0.004995
101.58	−0.0004	0.010492
101.6	0.008676	0.016839
101.62	0.007057	0.019061
101.64	−0.00287	0.010566
101.66	−0.01312	0.002488
101.68	−0.02369	−0.00073
101.7	0.005753	0.01568
101.72	−0.03254	−0.00466
101.74	0.001242	0.014457
101.76	−0.00255	0.013074
101.78	0.000222	0.017784
101.8	0.014923	0.025401
101.82	−0.00914	0.01277
101.84	−0.00271	0.007155
101.86	0.000434	0.018112
101.88	−0.01803	−0.00078
101.9	−0.01303	0.002261
101.92	−0.0082	0.01252
101.94	−0.01191	0.011698
101.96	−0.0139	0.007765
101.98	0.000233	0.013011
102	−0.02164	0.001753
102.02	−0.01144	0.010082
102.04	0.024934	0.033074
102.06	0.02058	0.028719
102.08	−0.00217	0.015068
102.1	−0.02279	−0.00178
102.12	0.01071	0.023104
102.14	−0.00659	0.014765
102.16	0.006528	0.019852
102.18	0.005214	0.021984
102.2	−0.00252	0.01579
102.22	0.011032	0.026308
102.24	−0.02418	0.005189
102.26	−0.01481	0.009586
102.28	−0.01232	0.011661
102.3	−0.00444	0.019197
102.32	−0.01985	0.011859
102.34	0.003785	0.027349
102.36	−0.00722	0.016842
102.38	−0.01821	0.008098
102.4	−0.0154	−0.0035
102.42	−0.00231	−0.00672
102.44	0.008561	−0.00995
102.46	0.023654	−0.00916
102.48	0.027756	−0.00688
102.5	−0.0056	−0.0234
102.52	0.020007	−0.0035
102.54	−0.00377	−0.00563
102.56	−0.00052	0.00088
102.58	−0.02149	−0.01682
102.6	−0.01192	0.009421
102.62	−0.00688	0.011326
102.64	−0.01577	0.004302
102.66	−0.0065	0.016879
102.68	−0.01563	0.005697
102.7	−0.00986	0.019887
102.72	−0.00648	0.014725
102.74	−0.0127	0.009003
102.76	−0.01673	−0.00292
102.78	−0.0091	−0.00829
102.8	0.010995	−0.0035
102.82	0.023401	−0.00055
102.84	0.016137	−0.00224
102.86	0.014258	−0.0055
102.88	0.020214	0.008698
102.9	0.002262	−0.00348
102.92	−0.00734	0.00147
102.94	−0.01204	0.001567
102.96	0.013766	0.024248
102.98	0.011548	0.010935
103	−0.00767	0.00947
103.02	0.002277	0.010909
103.04	−0.00268	0.01495
103.06	0.014563	0.02282
103.08	−0.00228	0.009512
103.1	−0.00848	0.005677
103.12	0.001457	0.01729
103.14	−0.02928	−0.00741
103.16	−0.00146	0.016224
103.18	0.000894	0.013234
103.2	0.010043	0.020246
103.22	0.017581	0.025632
103.24	0.005112	0.015947
103.26	−0.01533	0.006001
103.28	−0.00774	0.011085
103.3	0.002547	0.016729
103.32	−0.01757	−0.00266
103.34	0.004797	0.017696
103.36	−0.01248	0.005828
103.38	−0.02259	0.002359
103.4	−0.01627	0.00564
103.42	−0.014	0.005837
103.44	−0.01025	0.009629
103.46	0.020612	0.028264
103.48	−0.00651	0.013675
103.5	−0.01017	0.005929
103.52	0.022165	0.025516
103.54	−0.00054	0.01383
103.56	0.010574	0.01805
103.58	−0.015	0.003993
103.6	−0.00505	0.009703
103.62	−0.00791	0.007963
103.64	0.011568	0.022634
103.66	−0.00451	0.010203
103.68	−0.02726	−0.00169
103.7	0.002432	0.019483
103.72	−0.01933	0.006833
103.74	−0.01712	0.006514
103.76	−0.00327	0.008674
103.78	0.007754	0.02298
103.8	−0.00105	0.017256
103.82	−0.00204	0.015462
103.84	−0.01779	0.003513
103.86	−0.00126	0.016448
103.88	−0.0042	0.012736
103.9	0.024912	0.02706
103.92	−0.00162	0.016839
103.94	−0.0044	0.010535
103.96	−0.00904	0.012639
103.98	0.019292	0.026893
104	0.006823	0.016577
104.02	0.024846	0.027809
104.04	−0.00274	0.016858
104.06	−0.00606	0.016738
104.08	−0.01725	0.002008
104.1	−0.00271	0.00665
104.12	−0.01218	0.009649
104.14	−0.01267	0.004647
104.16	−0.01189	0.006343
104.18	0.006122	0.01759
104.2	0.001244	0.009688
104.22	−0.01046	0.006411
104.24	0.007301	0.017835
104.26	−0.00894	0.006875
104.28	−0.00219	0.014347
104.3	−0.01257	0.00906
104.32	−0.00129	0.013932
104.34	0.002277	0.014457
104.36	−0.02173	0.004884
104.38	−0.01135	0.002577
104.4	−0.00307	0.014301
104.42	0.013413	0.02538
104.44	0.017534	0.020664
104.46	−0.00498	0.012675
104.48	0.002742	0.012835
104.5	0.016579	0.025526
104.52	0.0163	0.025226
104.54	−0.01483	0.00426
104.56	−0.00117	0.014857
104.58	−0.00726	0.011542
104.6	0.019657	0.020512
104.62	0.005145	0.012631
104.64	0.010252	0.015038
104.66	−0.00437	0.010066
104.68	−0.00664	0.009872
104.7	−0.00302	0.01514
104.72	−0.00881	0.009691
104.74	0.013643	0.02061
104.76	−0.01097	0.004048
104.78	−0.01734	−0.00487
104.8	0.005059	0.020893
104.82	−0.02719	−0.00382
104.84	0.027941	0.027377
104.86	−0.02168	−0.00202
104.88	−0.00789	0.008775
104.9	−0.01106	0.007207
104.92	−0.01271	0.005004
104.94	−0.02582	−0.00081
104.96	−0.0091	0.008136
104.98	−0.01127	0.004315
105	−0.00952	0.009554
105.02	0.014727	0.026915
105.04	−0.01203	0.004252
105.06	−0.00101	0.015911
105.08	−0.01147	0.006287
105.1	0.008048	0.016688
105.12	−0.00259	0.012667
105.14	−0.01152	0.005486
105.16	−0.00556	0.014273
105.18	−0.02094	0.001476
105.2	−0.00773	0.003711
105.22	−0.00493	0.015045
105.24	0.01473	0.023606
105.26	−0.02534	−0.00441
105.28	0.009817	0.018103
105.3	0.002523	0.01538
105.32	−0.01831	0.002874
105.34	−0.00515	0.01166
105.36	−0.00583	0.01013
105.38	−0.00556	0.013808
105.4	0.022348	0.02419
105.42	0.000701	0.018064
105.44	−0.00345	0.007818
105.46	−0.01037	0.007088
105.48	−0.0088	0.0088
105.5	0.016801	0.021943
105.52	−0.00726	0.006799
105.54	−0.01662	0.000558
105.56	−0.00888	0.008363
105.58	−0.02103	0.004491
105.6	−0.00695	0.004723
105.62	−0.01978	0.002071
105.64	−0.01433	0.002527
105.66	−0.00086	0.013849
105.68	−0.01724	0.002792
105.7	−0.00682	0.009814
105.72	0.01154	0.024135
105.74	0.006792	0.01505
105.76	−0.00051	0.016171
105.78	−0.00798	0.015024
105.8	−0.01467	0.005263
105.82	−0.00021	0.013471
105.84	−0.01281	0.007098
105.86	−0.00287	0.012804
105.88	−0.01304	0.009589
105.9	−0.0194	0.001311
105.92	−0.01548	0.00271
105.94	0.003044	0.011975
105.96	−0.00311	0.008514
105.98	0.01027	0.018259
106	−0.02273	−0.00077
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106.04	−0.00448	0.014334
106.06	−0.00705	0.008191
106.08	−0.00778	0.008699
106.1	−0.00543	0.010619
106.12	−0.00708	0.002089
106.14	0.0171	0.024275
106.16	0.006664	0.013506
106.18	−0.01212	0.008006
106.2	0.013315	0.023662
106.22	0.001964	0.015711
106.24	0.001313	0.015264
106.26	−0.00615	0.012186
106.28	0.006127	0.01508
106.3	0.013736	0.023342
106.32	−0.02336	−0.00762
106.34	−0.01143	0.006585
106.36	−0.02982	−0.00649
106.38	−0.00669	0.01116
106.4	0.006944	0.018564
106.42	0.025858	0.032099
106.44	−0.01025	0.005792
106.46	0.015935	0.023187
106.48	−0.00641	0.008815
106.5	−0.00926	0.010544
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106.6	−0.01159	0.007252
106.62	−0.007	0.009798
106.64	−0.01539	0.006324
106.66	−0.00161	0.010584
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106.7	0.019713	0.019549
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106.74	0.012828	0.020598
106.76	−0.00224	0.018031
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106.8	0.019824	0.022045
106.82	−0.01073	0.001944
106.84	0.002943	0.016006
106.86	−0.00795	0.011769
106.88	0.019316	0.023791
106.9	−0.00512	0.008858
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106.94	−0.00798	0.012767
106.96	−0.00589	0.011593
106.98	0.015292	0.017064
107	−0.02189	−0.00096
107.02	0.001306	0.018677
107.04	−0.02379	−9.9E−05
107.06	0.015543	0.021567
107.08	0.016741	0.0219
107.1	−0.01182	0.009646
107.12	0.007324	0.015652
107.14	−0.01597	0.002459
107.16	−0.01302	0.001835
107.18	−0.01422	−0.00119
107.2	−0.00784	0.013004
107.22	0.00469	0.01752
107.24	0.008393	0.017361
107.26	0.001263	0.006118
107.28	0.000093	0.01587
107.3	0.001317	0.013097
107.32	−0.00214	0.00954
107.34	0.004762	0.013939
107.36	−0.00895	0.006936
107.38	0.002873	0.018754
107.4	−0.0231	0.002322
107.42	−0.01749	0.003518
107.44	0.007306	0.015903
107.46	−0.00648	0.010782
107.48	0.009974	0.022881
107.5	−0.00434	0.012366
107.52	−0.01813	0.00077
107.54	−0.00476	0.011603
107.56	0.008645	0.015635
107.58	−0.01116	0.01196
107.6	−0.01174	0.004426
107.62	−0.01181	0.010725
107.64	−0.00267	0.015647
107.66	−0.00396	0.005611
107.68	0.013904	0.023095
107.7	0.015494	0.025259
107.72	−0.00875	0.011387
107.74	0.000734	0.013469
107.76	−0.00516	0.007431
107.78	0.006383	0.016171
107.8	0.001612	0.01599
107.82	−0.00656	0.004029
107.84	0.004053	0.013097
107.86	−0.00683	0.009138
107.88	−0.00353	0.00799
107.9	−0.009	0.002188
107.92	−0.00434	0.014196
107.94	0.013879	0.017398
107.96	−0.00471	0.008151
107.98	−0.0053	0.011018
108	−0.00028	0.014324
108.02	−0.0225	0.0024
108.04	0.013148	0.01979
108.06	−0.00057	0.013129
108.08	−0.01603	0.007563
108.1	0.017029	0.021085
108.12	−0.02203	−0.00374
108.14	−0.02152	0.001365
108.16	0.009679	0.014384
108.18	0.01137	0.018989
108.2	0.0147	0.022243
108.22	−0.00767	0.009788
108.24	0.007415	0.015997
108.26	−0.00933	0.014438
108.28	−0.02639	−0.00322
108.3	0.009964	0.02262
108.32	0.012484	0.023717
108.34	−0.0006	0.012025
108.36	0.016505	0.015613
108.38	−0.00459	0.006864
108.4	0.005136	0.018213
108.42	0.004779	0.015407
108.44	−0.00664	0.006897
108.46	0.010687	0.014099
108.48	−0.01282	0.008643
108.5	0.00435	0.01688
108.52	−0.0068	0.008414
108.54	−0.00787	0.005601
108.56	−7.3E−05	0.013434
108.58	0.004902	0.013033
108.6	0.005983	0.019497
108.62	0.000281	0.012543
108.64	0.015066	0.015597
108.66	0.011898	0.020802
108.68	−0.03065	−0.00958
108.7	−0.02216	−0.00055
108.72	−0.00305	0.012811
108.74	−0.01067	0.002516
108.76	−0.0094	0.009585
108.78	−0.00223	0.012391
108.8	−0.00184	0.009704
108.82	0.000667	0.013547
108.84	−0.00081	0.014426
108.86	−0.00124	0.012673
108.88	−0.01167	0.012171
108.9	−0.00651	0.005464
108.92	−0.0072	0.005285
108.94	0.000861	0.014206
108.96	−0.00153	0.011107
108.98	0.001541	0.013965
109	0.010388	0.019182
109.02	−0.00213	0.012545
109.04	−0.02775	−0.01038
109.06	−0.00837	0.003427
109.08	−0.01041	0.006098
109.1	0.011133	0.017993
109.12	−0.01195	0.00976
109.14	0.002812	0.013271
109.16	0.016881	0.026923
109.18	0.027616	0.026246
109.2	0.003956	0.016516
109.22	−0.00622	0.010415
109.24	−0.02133	−0.00122
109.26	−0.00439	0.008423
109.28	0.006537	0.022502
109.3	−0.01852	0.000284
109.32	−0.01076	0.006959
109.34	0.000146	0.014272
109.36	0.008017	0.020842
109.38	0.01654	0.022687
109.4	−0.01611	0.010173
109.42	−0.03907	−0.00938
109.44	−0.0107	0.007298
109.46	0.000642	0.015886
109.48	0.001855	0.016886
109.5	0.001051	0.009562
109.52	0.006437	0.018612
109.54	−0.01005	0.010844
109.56	0.000861	0.011649
109.58	0.002925	0.016154
109.6	−0.0064	0.012997
109.62	0.0001	0.015759
109.64	0.004502	0.016945
109.66	−0.02	−0.00016
109.68	0.043661	0.0421
109.7	0.01026	0.018294
109.72	−0.00713	0.008635
109.74	−0.01071	0.010445
109.76	0.017508	0.025596
109.78	−0.00645	0.017104
109.8	0.030086	0.030517
109.82	−0.00374	0.013523
109.84	−0.00598	0.008651
109.86	−0.00203	0.008283
109.88	−0.00794	0.001118
109.9	−0.01771	0.004041
109.92	−0.00503	0.009698
109.94	−0.00659	0.008546
109.96	−0.01547	0.00564
109.98	−0.03487	−0.01033
110	0.004511	0.013785
110.02	−0.01145	0.004403
110.04	0.006491	0.017589
110.06	0.004947	0.014058
110.08	−0.0142	0.0088
110.1	0.006904	0.021072
110.12	−0.01271	0.005093
110.14	−0.03184	−0.0064
110.16	−0.00327	0.008333
110.18	0.001689	0.012681
110.2	−0.00977	0.008915
110.22	−0.00121	0.007769
110.24	−0.00596	0.00734
110.26	0.004992	0.015123
110.28	−0.011	0.011551
110.3	−0.0089	0.007936
110.32	0.006331	0.019944
110.34	−0.00018	0.016992
110.36	−0.00632	0.014165
110.38	−0.00721	0.011609
110.4	−0.03421	−0.00494
110.42	−0.00257	0.019217
110.44	−0.01821	0.004355
110.46	0.003866	0.018891
110.48	0.001266	0.02082
110.5	−0.0025	0.016721
110.52	−0.00673	0.011936
110.54	−0.02095	0.000701
110.56	−0.00927	0.002971
110.58	−0.00173	0.004945
110.6	0.004059	−0.00222
110.62	0.01152	−0.00629
110.64	0.011658	−0.01217
110.66	0.019506	−0.01229
110.68	0.022104	−0.00935
110.7	0.018721	−0.01065
110.72	0.009086	−0.01367
110.74	−0.00058	−0.01713
110.76	−0.01119	−0.01299
110.78	0.00222	0.000703
110.8	0.010714	0.007021
110.82	−0.02093	−0.00747
110.84	0.003557	0.011956
110.86	−0.00173	0.011364
110.88	−0.01124	0.006089
110.9	−0.01476	0.004969
110.92	0.014183	0.021626
110.94	−4.4E−05	0.016399
110.96	−0.01326	0.005051
110.98	−0.00628	0.007444
111	0.002718	0.004715
111.02	0.004194	−0.00091
111.04	0.003605	−0.0084
111.06	0.008828	−0.01132
111.08	0.012139	−0.01184
111.1	0.000791	−0.01718
111.12	0.001154	−0.01234
111.14	0.000201	−0.01274
111.16	0.040682	0.020824
111.18	0.003197	0.004108
111.2	0.014866	0.010329
111.22	0.010559	0.006824
111.24	−0.00243	0.006253
111.26	0.031436	0.027297
111.28	0.001321	0.011124
111.3	0.004311	0.014182
111.32	−0.00011	0.01035
111.34	0.002336	0.010285
111.36	−0.01363	0.01299
111.38	−0.00353	0.010108
111.4	0.007371	0.009028
111.42	0.010059	0.017424
111.44	−0.02126	−0.00365
111.46	−0.00838	0.006878
111.48	−0.00957	0.009255
111.5	0.00548	0.017768
111.52	−0.01385	0.003921
111.54	−0.01056	0.005973
111.56	−0.00384	0.01394
111.58	−0.01418	0.000823
111.6	0.000128	0.011199
111.62	−0.01395	0.004233
111.64	0.002856	0.010183
111.66	0.010811	0.019661
111.68	−0.00989	0.00606
111.7	−0.00492	0.011221
111.72	−0.00407	0.013282
111.74	0.004195	0.018405
111.76	−0.0219	0.005153
111.78	−0.01083	0.008246
111.8	−0.00839	0.010944
111.82	0.002997	0.010201
111.84	0.004185	0.01748
111.86	0.016719	0.022698
111.88	0.003362	0.018104
111.9	0.000533	0.017458
111.92	−0.02005	0.00146
111.94	−0.03067	−0.00323
111.96	−0.00076	0.018877
111.98	−0.01122	0.012175
112	0.003265	0.017306
112.02	−0.02818	−0.00079
112.04	−0.01674	0.012315
112.06	−0.02927	0.00044
112.08	−0.01888	0.012586
112.1	−0.01729	0.005078
112.12	−0.01447	0.002822
112.14	−0.00551	0.000109
112.16	−0.0076	−0.01032
112.18	0.006828	−0.0111
112.2	0.009259	−0.01554
112.22	0.0092	−0.01987
112.24	0.020594	−0.01176
112.26	0.002946	−0.01989
112.28	0.0159	−0.00995
112.3	0.01301	0.000528
112.32	−0.01174	−0.00736
112.34	−0.00475	−0.00504
112.36	0.021828	0.021778
112.38	−0.01065	0.004502
112.4	−0.01871	−0.00092
112.42	−0.00811	0.005971
112.44	0.017433	0.017259
112.46	−0.01197	0.008293
112.48	−0.01705	0.002527
112.5	−0.01034	0.01225
112.52	−0.02496	0.00409
112.54	−0.02216	0.002684
112.56	−0.01646	−0.00091
112.58	−0.00293	−0.00126
112.6	−0.00414	−0.00906
112.62	0.016701	−0.00647
112.64	0.007807	−0.01077
112.66	0.00975	−0.01004
112.68	0.018665	−0.00224
112.7	0.011331	−0.00786
112.72	−0.00835	−0.01206
112.74	−0.00271	−0.00319
112.76	0.001857	0.001638
112.78	0.019464	0.017116
112.8	0.004835	0.004366
112.82	−0.0196	−0.00872
112.84	−0.00472	0.008354
112.86	0.001913	0.014051
112.88	0.014956	0.020161
112.9	−0.01775	0.000247
112.92	−0.01571	0.005424
112.94	−0.00275	0.008243
112.96	−0.00031	0.006547
112.98	0.000442	0.010156
113	0.015333	0.014285
113.02	−0.02237	−0.00359
113.04	0.002976	0.015847
113.06	−0.00698	0.006044
113.08	0.028104	0.034773
113.1	0.008071	0.022023
113.12	0.000704	0.015425
113.14	0.018846	0.026526
113.16	−0.00158	0.009554
113.18	−0.00792	0.007152
113.2	0.000825	0.016994
113.22	0.000695	0.010121
113.24	−0.02656	0.00115
113.26	0.023904	0.029794
113.28	−0.03	−0.006
113.3	−0.00074	0.016641
113.32	−0.01678	0.010706
113.34	0.000781	0.017067
113.36	−0.02785	0.001865
113.38	−0.02835	0.001224
113.4	−0.0281	0.003387
113.42	−0.00698	0.017486
113.44	−0.02462	0.005697
113.46	−0.01858	0.005584
113.48	−0.00813	0.007193
113.5	−0.01018	0.000089
113.52	0.006851	−0.00234
113.54	−0.00488	−0.01341
113.56	0.005681	−0.00639
113.58	0.012402	0.00389
113.6	−0.00928	0.002108
113.62	−0.00698	0.014428
113.64	−0.03049	0.001799
113.66	−0.01197	0.019535
113.68	−0.01168	0.015001
113.7	−0.01482	0.008379
113.72	−0.00412	0.004937
113.74	−0.00193	−0.00527
113.76	0.007295	−0.01145
113.78	0.009193	−0.0137
113.8	0.007872	−0.0128
113.82	−0.00197	−0.01554
113.84	−0.00596	−0.01063
113.86	0.012074	0.008671
113.88	−0.0033	0.001871
113.9	−0.00401	0.008458
113.92	−9.5E−05	0.005905
113.94	0.020134	0.024864
113.96	0.023386	0.016142
113.98	0.007707	0.005338
114	0.015248	0.009513
114.02	−0.00063	0.003426
114.04	−0.00246	0.009008
114.06	−0.02391	0.002053
114.08	−0.0038	0.019147
114.1	−0.01612	0.016284
114.12	−0.03381	0.001946
114.14	−0.01752	0.005157
114.16	−0.01076	0.006153
114.18	−0.01778	−0.00941
114.2	−0.00941	−0.01538
114.22	−0.00269	−0.00857
114.24	0.014161	0.001434
114.26	0.022701	0.008857
114.28	0.00234	−0.0026
114.3	−0.02732	−0.01569
114.32	−0.00127	0.008876
114.34	−0.00233	0.000669
114.36	−0.00592	0.003912
114.38	−0.0009	0.006057
114.4	−0.00793	0.005211
114.42	−0.00168	0.011683
114.44	0.000866	0.014732
114.46	0.011709	0.0197
114.48	0.000493	0.0159
114.5	0.010365	0.020723
114.52	−0.01247	0.003169
114.54	0.006943	0.016898
114.56	−0.01713	0.003394
114.58	−0.0181	0.005559
114.6	−0.01272	0.006538
114.62	−0.02533	−0.00217
114.64	−0.02091	0.00323
114.66	−0.0148	0.007832
114.68	−0.00827	0.010341
114.7	−0.0012	0.020374
114.72	−0.00443	0.017612
114.74	−0.0114	0.016936
114.76	−0.01763	0.014063
114.78	−0.02618	0.010446
114.8	−0.01892	0.010584
114.82	−0.02255	0.005252
114.84	−0.02922	−0.00338
114.86	−0.01562	−0.00913
114.88	0.00142	−0.00874
114.9	0.005365	−0.01099
114.92	0.007525	−0.01095
114.94	0.013741	−0.0089
114.96	0.00303	−0.00543
114.98	0.005568	0.000261
115	−0.01737	−0.01281
115.02	−0.01166	−0.00669
115.04	−0.00673	0.003316
115.06	−0.00604	0.00339
115.08	0.002793	0.016765
115.1	−0.00422	0.00912
115.12	0.029091	0.030351
115.14	−0.01021	0.010405
115.16	−0.01479	0.004536
115.18	−0.01418	0.013757
115.2	−0.03516	0.000195
115.22	−0.02597	0.009107
115.24	−0.02972	0.007761
115.26	−0.0267	0.007191
115.28	−0.01963	0.006741
115.3	−0.00667	0.007116
115.32	−0.01628	−0.0014
115.34	0.001505	0.00687
115.36	0.029066	0.012849
115.38	0.022405	0.007828
115.4	−0.00972	−0.01348
115.42	−0.02371	−0.014
115.44	−0.00234	0.000688
115.46	−0.00356	0.001133
115.48	0.01286	0.012723
115.5	−0.00086	0.005322
115.52	−0.00709	0.002517
115.54	−0.02858	−0.00978
115.56	−0.00294	0.006817
115.58	−0.00759	0.007778
115.6	0.00733	0.014095
115.62	−0.01126	0.00232
115.64	−0.0196	−0.00093
115.66	−0.01618	−0.00509
115.68	−0.00449	0.012252
115.7	−0.00639	0.013448
115.72	−0.00095	0.011876
115.74	−0.01181	0.011515
115.76	0.009835	0.019288
115.78	−0.00764	0.013829
115.8	−0.01554	0.00414
115.82	−0.01419	0.002282
115.84	−0.00577	0.001259
115.86	−0.00288	0.012564
115.88	0.007301	0.021897
115.9	0.009503	0.022772
115.92	−0.00286	0.008301
115.94	0.018627	0.020388
115.96	0.0089	0.017314
115.98	−0.00176	0.01311
116	0.002824	0.010493
116.02	−0.0201	0.000912
116.04	0.007664	0.017786
116.06	0.010643	0.015276
116.08	0.008188	0.018606
116.1	0.015788	0.018025
116.12	−0.01705	0.000792
116.14	0.000722	0.013726
116.16	−0.0028	0.012667
116.18	0.013398	0.019907
116.2	−0.02878	−0.00468
116.22	−0.00822	0.003935
116.24	−0.00783	0.007435
116.26	0.00473	0.012519
116.28	−0.0004	0.008212
116.3	−0.00574	0.011773
116.32	−0.00411	0.009648
116.34	−0.01694	0.002887
116.36	−0.01405	−0.00021
116.38	−0.00694	0.010765
116.4	−0.00927	0.006003
116.42	0.00003	0.014622
116.44	−0.00682	0.00809
116.46	−0.00392	0.012412
116.48	0.005112	0.017002
116.5	−0.0072	0.009519
116.52	0.000129	0.01605
116.54	−0.02364	0.004833
116.56	−0.01894	0.000501
116.58	−0.01009	0.010915
116.6	−0.00361	0.014601
116.62	−0.00017	0.012688
116.64	−0.01199	0.003298
116.66	−0.00421	0.009629
116.68	−0.00668	0.004538
116.7	−0.00819	0.011062
116.72	−0.02306	0.001598
116.74	−0.00081	0.01036
116.76	0.003101	0.016547
116.78	0.014171	0.023757
116.8	−0.0161	−0.00113
116.82	0.007129	0.013013
116.84	−0.02666	−0.0068
116.86	0.014072	0.019135
116.88	−2.1E−05	0.005092
116.9	−0.00918	0.007014
116.92	−0.02245	0.001916
116.94	0.001255	0.013821
116.96	0.007116	0.016323
116.98	−0.02343	−0.00575
117	−0.01921	0.003213
117.02	−0.00847	0.009964
117.04	−0.0094	0.011505
117.06	−0.00783	0.010725
117.08	−0.0054	0.007852
117.1	0.015583	0.024956
117.12	−0.02235	0.001927
117.14	−0.01175	0.006537
117.16	−0.00225	0.014178
117.18	−0.00665	0.015866
117.2	−0.0061	0.016445
117.22	−0.01037	0.013483
117.24	0.000083	0.018578
117.26	−0.01148	0.012896
117.28	−0.02023	0.007741
117.3	−0.00162	0.017161
117.32	−0.01376	0.011954
117.34	−0.00807	0.017453
117.36	−0.01227	0.013651
117.38	−0.01316	0.011214
117.4	−0.02737	0.001063
117.42	−0.01725	0.011102
117.44	−0.02083	0.012708
117.46	−0.02744	0.007306
117.48	−0.03965	−0.00446
117.5	−0.01416	0.016204
117.52	−0.03427	0.003661
117.54	−0.03547	0.000591
117.56	−0.03475	−0.00045
117.58	−0.02219	0.001408
117.6	−0.00887	0.001999
117.62	−0.00806	−0.00898
117.64	0.000098	−0.01125
117.66	0.012757	−0.01294
117.68	0.014287	−0.01728
117.7	0.013474	−0.01888
117.72	0.002099	−0.02524
117.74	0.002039	−0.0261
117.76	−0.00619	−0.02362
117.78	0.010354	−0.01003
117.8	−0.00926	−0.01989
117.82	−0.01482	−0.01112
117.84	−0.00147	0.000988
117.86	−0.00406	0.003591
117.88	−0.01675	−0.00263
117.9	−0.01413	0.006744
117.92	−0.02431	−0.00116
117.94	−0.01533	0.01011
117.96	−0.01729	0.010427
117.98	−0.01411	0.013697
118	−0.02792	0.007176
118.02	−0.0308	0.005481
118.04	−0.03761	−0.00118
118.06	−0.02366	−0.0009
118.08	−0.0124	−0.00158
118.1	−0.00641	−0.00618
118.12	−0.00316	−0.01559
118.14	0.012606	−0.01158
118.16	0.002479	−0.0222
118.18	0.011127	−0.015
118.2	−0.00254	−0.02292
118.22	−9.9E−05	−0.01557
118.24	0.00157	−0.01289
118.26	0.006153	−0.0058
118.28	0.022332	0.011982
118.3	−0.01499	−0.01249
118.32	0.003481	0.007818
118.34	−0.02536	−0.01586
118.36	−0.00987	0.005366
118.38	0.007152	0.008617
118.4	−0.02708	−0.00628
118.42	0.01761	0.020169
118.44	0.008643	0.020609
118.46	0.003394	0.011489
118.48	−0.00694	−0.00232
118.5	0.013065	0.019702
118.52	−0.00151	0.006542
118.54	−0.009	0.008803
118.56	0.002038	0.013202
118.58	0.011616	0.020439
118.6	−0.00241	0.013868
118.62	0.013087	0.020164
118.64	0.005878	0.014292
118.66	−0.00471	0.006552
118.68	0.000833	0.014114
118.7	−0.00358	0.00867
118.72	−0.00164	0.005902
118.74	0.009686	0.011759
118.76	0.002378	0.007294
118.78	−0.00507	0.00754
118.8	−0.00858	0.004964
118.82	−0.01092	0.003122
118.84	0.005075	0.013621
118.86	−0.0195	−0.00649
118.88	0.023209	0.02222
118.9	0.015314	0.023298
118.92	−0.00688	0.004848
118.94	−0.01062	0.006513
118.96	0.006225	0.014126
118.98	−0.01323	0.006357
119	−0.01464	0.005723
119.02	−0.01396	0.004828
119.04	0.009927	0.020719
119.06	−0.00086	0.010196
119.08	−0.01956	0.003068
119.1	−0.01526	0.006848
119.12	−0.00488	0.01893
119.14	0.000693	0.020902
119.16	0.003719	0.014355
119.18	−0.02016	−0.00035
119.2	−0.01557	0.008493
119.22	−0.01252	0.011614
119.24	−0.03059	0.001387
119.26	−0.01591	0.009152
119.28	−0.00636	0.015349
119.3	−0.01812	0.011047
119.32	−0.02775	0.009686
119.34	−0.03205	0.004938
119.36	−0.02416	0.012604
119.38	−0.03136	0.008209
119.4	−0.02603	0.01094
119.42	−0.02574	0.011938
119.44	−0.02573	0.010883
119.46	−0.02278	0.00714
119.48	−0.02336	−0.00179
119.5	−0.00678	−0.00024
119.52	−0.00097	−0.00812
119.54	0.015825	−0.00462
119.56	0.018466	−0.00822
119.58	0.018802	−0.00995
119.6	0.014315	−0.00994
119.62	0.00665	−0.00816
119.64	−0.00584	−0.01002
119.66	0.008738	0.001698
119.68	0.000506	−0.00251
119.7	−0.0047	0.001826
119.72	−0.00332	0.004063
119.74	−0.00352	0.002677
119.76	−0.00102	0.011956
119.78	−0.00734	0.011878
119.8	−0.00711	0.008634
119.82	−0.00715	0.012202
119.84	−0.01411	0.007991
119.86	−0.02427	0.007381
119.88	−0.01962	0.013027
119.9	−0.02421	0.011376
119.92	−0.02752	0.01389
119.94	−0.02228	0.015415
119.96	−0.01885	0.008414
119.98	−0.00649	0.009735
120	0.001124	0.008883

[0034] The lithium cobalt oxides of the present invention are prepared by first mixing together one or more lithium source compounds, one or more cobalt source compounds, and one or more source compounds that include the dopants A in the desired stoichiometric amounts to produce lithium cobalt oxides having the formula LiwCo1−xAxO2+y wherein 0.96≦w≦1.05, 0≦x≦0.05, −0.02≦y≦0.02. The source compounds (raw materials) can be the pure elements but are typically compounds containing the elements such as oxides or salts thereof. For example, the source compounds are typically hydrated or anhydrous oxides, hydroxides, carbonates, nitrates, sulfates, chlorides or fluorides, but can be any other suitable source compound that will not cause elemental defects in the resulting lithium cobalt oxide compound. The elements for the lithium cobalt oxide compound can each be supplied from separate source compounds or at least two of the elements can be supplied from the same source compounds. In addition, the source compounds can be mixed in any desirable order.

[0035] Although the lithium cobalt oxide compounds are preferably prepared by solid state reactions (i.e. dry mixing), it can be advantageous to react the raw materials using wet chemistry such as sol-gel type reactions or spray drying techniques, alone or in combination with solid state reactions. For example, the cobalt and dopant source compounds can be prepared as a solution in a solvent such as water and the cobalt and dopants precipitated out of solution as an intimately mixed compound such as a hydroxide. The mixed compound can then be blended with a lithium source compound. The reaction mixture can also be prepared by suspending source compounds in a solution of other source compounds and spray drying the resulting slurry to obtain an intimate mixture. Typically, the selection of reaction methods will vary depending on the raw materials used and the desired end product. Preferably, in accordance with the present invention, the lithium source compound is selected from the group consisting of Li2CO3 and LiOH and the cobalt source compound is selected from the group consisting of Co3O4 and Co(OH)2.

[0036] The mixture of source compounds once prepared can be reacted to form the lithium metal oxide. The source compounds are reacted by heating (i.e. firing) the source compounds in a first heating step at a temperature below about 850° C., preferably from about 500° C. to about 850° C., to produce the LiwCo1−xAxO2+y compound. The source compounds are heated for a period of time sufficient to react the source compounds to produce a LiwCo1−xAxO2+y compound that is substantially free of lithium and cobalt phases. Preferably, the source compounds are heated for a period of time of from about 30 minutes to about 3 hours to produce the LiwCo1−xAxO2+y compound. The source compounds can also be heated in the first heating step at more than one temperature within the above temperature range and time period. For example, the source compounds can be heated for 1 hour at 600° C. and for 1 hour at 700° C. to produce the lithium cobalt oxides. Typically, the temperature and time period used in the first heating step is dependent on the raw material used and the desired grain size for the resulting lithium cobalt oxide compound. In particular, larger grain sizes (e.g. 10 microns) can require longer heating times.

[0037] Once the LiwCo1−xAxO2+y compounds are produced, these compounds are heated in a second heating step at a temperature from about 900° C. and 1000° C., preferably from about 950° C. to about 980° C., to form and enhance the hexagonal layered crystal structure of these compounds. The LiwCo1−xAxO2+y compound is preferably heated in the second heating step for a period of time of from about 30 minutes to about 7 hours. The LiwCo1−xAxO2+y compound can also be heated in the second heating step at more than one temperature within the above range and time period. Typically, the temperature and time period used for the second heating step is dependent on the grain size of the lithium cobalt oxide compound.

[0038] Any suitable apparatus can be used for heating or firing the mixture, such as a rotary calciner, a stationary furnace or a tunnel furnace, that uniformly heats the source compounds (first heating step) or the lithium cobalt oxide (second heating step) to produce the lithium cobalt oxides. Preferably, a rotary calciner is used in accordance with the invention. In addition, any suitable atmosphere such as air and other oxygen-containing atmospheres can be used in accordance with the invention as long as the atmosphere provides the desired oxygen content to form the lithium cobalt oxides.

[0039] Once the lithium cobalt oxide is at its final preparation temperature, the lithium cobalt oxide is preferably cooled at a rate of from about 8° C./min to about 140° C./min, more preferably from about 110° C./min to 100° C./min. Cooling at a rate of greater than 140° C./min undesirably produces a structure with high crystalline stress and strain that does not have the strength of lithium cobalt oxides cooled at a rate of between 8° C./min and 140° C./min. Moreover, cooling at a rate of less than 8° C./min undesirably results in the formation of localized cubic spinel-like structural phases on the surface of the crystal or within the crystal and thus decreased electrochemical performance. With the lithium cobalt oxides of the invention, the lack of localized hetero-structural phases, e.g., cubic spinel-like phases, within the crystal and on the crystal surface does not induce further phase transformation that impedes the diffusion of the Li+ ions during the charge and discharge cycles. Thus, the hexagonal layered compounds of the invention have better and more consistent electrochemical performance than prior art compounds that are cooled at slower rates.

[0040] The lithium cobalt oxide is preferably uniformly cooled (i.e. quenched) in accordance with the invention. In particular, the lithium cobalt oxide material is preferably cooled at approximately the same rate. For example, the variation between the mean cooling rate and the cooling rate for any specific portion of the material should be less than about 10 percent. In a preferred embodiment of the invention, uniform cooling can be accomplished using a rotary calciner, or a stationary furnace or tunnel furnace with smaller bed depths. The uniformly cooled material prepared according to the invention has greater homogeneity and less variance in its material properties than material that is not uniformly cooled.

[0041] The present invention further includes rechargeable lithium and lithium ion secondary batteries that include a positive electrode comprising the lithium cobalt oxides of the invention. Typically, the lithium cobalt oxide compound of the invention is combined with a carbonaceous material and a binder polymer to form a cathode. The negative electrode of the lithium battery can be lithium metal or alloys, or any material capable of reversibly lithiating and delithiating at an electrochemical potential relative to lithium metal between about 0.0 V and 0.7 V. Examples of negative electrode materials include carbonaceous materials containing H, B, Si and Sn; tin oxides; tin-silicon oxides; and composite tin alloys. The negative electrode is separated from the positive electrode material in the cell using an electronic insulating separator. The electrochemical cell further includes an electrolyte. The electrolyte can be non-aqueous liquid, gel or solid and preferably comprises a lithium salt, e.g., LiPF6. Electrochemical cells using the lithium cobalt oxide compounds of the invention as positive electrode material can be combined for use in portable electronics such as cellular phones, camcorders, and laptop computers, and in large power applications such as for electric vehicles and hybrid electric vehicles.

[0042] The lithium cobalt oxide compounds of the invention allow lithium ions to readily diffuse during both the charge and discharge cycles of the battery. In particular, in the charge cycle for these lithium cobalt oxides wherein z Li per formula unit are electrochemically removed per formula unit, the lithium cobalt oxide takes the formula Liw-zCo1−xAxO2+y, wherein 0≦z≦w.

[0043] The present invention further includes a method of analyzing a compound to determine if the compound is suitable for use as the active positive electrode material in a lithium or lithium-ion secondary battery. The method of the invention comprises determining a principal component space defined by the relationship axi+byi≦c, wherein xi={right arrow over (S)}i·{right arrow over (P)}c1; yi={right arrow over (S)}i·{right arrow over (P)}c2; the vector {right arrow over (S)}i is the x-ray spectrum for the compound; the vectors {right arrow over (P)}c1 and {right arrow over (P)}c2 are determined by measuring the x-ray powder diffraction values {right arrow over (S)}i for a predetermined range of 2θ values using a predetermined step size by sampling a plurality of samples of compounds having the same general formula as the compound and using the regression of {right arrow over (S)}i of the sample set against predetermined battery performance data for the samples by incorporating the samples as the positive electrode active material in a lithium or lithium-ion secondary battery. The xi and yi values for the compounds in the sample set that have the predetermined battery performance data are then used to determine a, b and c. The compound is analyzed by measuring the x-ray diffraction spectra for the compound to obtain x and y values and determining whether the x and y values meet the relationship axi+byi≦c. If the x and y values meet this relationship, the compound will possess the battery performance and x-ray diffraction spectra suitable for use as the active positive electrode material (as defined by the predetermined battery performance values).

[0044] In accordance with the method of analysis described in accordance with the invention, it is important that the compounds in the sample set have the same general formula as the compound being tested. In addition, it is important that the compounds be tested using the same conditions to provide consistent and reliable results. The positive electrode active materials tested using the method of the invention can be any of those known in the art and are preferably lithiated. Preferably, the compound is a compound selected from the group consisting of doped and undoped lithium nickel oxides, lithium cobalt oxides and lithium manganese oxides, and more preferably it is lithium cobalt oxide as discussed above. Different battery performance properties (e.g. fade, specific capacity, and the like), and different thresholds for these properties can be used to determine the principal component space. Preferably, the samples that are used to determine the principal component space are selected based on meeting a threshold predetermined capacity fade after a predetermined number of cycles under predetermined cycling conditions. For example, as discussed above, the predetermined range of 2θ values can be between 15° and 120° using CuKα rays, the predetermined step size can be 0.02°, and the predetermined capacity fade after 50 cycles of a lithium coin cell that includes a lithium negative electrode and the lithium cobalt oxide as the positive electrode material and that is cycled between 3.0 and 4.3V at a constant current of C/3 during both charge and discharge cycles can be less than or equal to 15%. More preferably, the principal component space is defined by the relationship xi+0.77 yi≦−6. Although different methods can be used to determine the regression of {right arrow over (S)}i of the sample set, the regression is preferably determined using a partial least squares regression method as discussed above.

[0045] The present invention will now be further demonstrated by the following non-limiting examples.

EXAMPLES

[0046] Sample Preparation:

[0047] Stoichiometric amounts of Li2CO3 and Co3O4 with about 2 molar percent in lithium excess were thoroughly mixed and then fired in air as follows:

[0048] Sample S1 was heated at a rate of about 18° C./min from room temperature to 750° C., held at 750° C. for 1 hour, then heated to 950° C. in about 10 minutes, and held at 950° C. for 4 hours, followed by a rapid cooling to room temperature in about 10 minutes.

[0049] Sample S2 was heated at a rate of about 18° C./min from room temperature to 800° C., held at 800° C. for 1 hour, then heated to 975° C. in about 10 minutes, and held at 975° C. for 4 hours, followed by a rapid cooling to room temperature in about 10 minutes.

[0050] Sample S3 was heated at a rate of about 5° C./min from room temperature to 800° C., held at 800° C. for 3 hour, then heated to 975° C. in about 1 hour, and held at 975° C. for 9 hours, followed by a cooling to room temperature at a rate of about 5° C./min.

[0051] Sample S4 was heated at a rate of about 25° C./min from room temperature to 800° C., held at 800° C. for 30 min, then heated to 975° C. in about 10 min, and held at 975° C. for 2 hours, followed by a rapid cooling to room temperature in about 30 minutes.

[0052] Comparative sample CS1 was heated at a rate of 3.75° C./min from room temperature to 950° C., held at 950° C. for 5 hours, followed by a cooling to room temperature at a rate of 3.75° C./min.

[0053] Coin Cell Testing:

[0054] NRC 2325 coin cell hardware and Celgard 3501 separators were used. The electrolyte was 1M LiPF6 in a 50:50 mixture of ethylene carbonate and dimethyl carbonate solvents. The positive electrode consisted of about 85% active material (by weight), 10% Super S™ carbon black and 5% polyvinylidene fluoride (PVDF) as a binder polymer, coated on aluminum foil. The negative electrode was metallic lithium foil. The cell was cycled between 3.0 and 4.3V at a constant current of C/3 (3 hours for complete charge or discharge) during both the charge and discharge cycles.

[0055] X-Ray Diffraction:

[0056] A Rigaku RINT-2000 unit that included a graphite monochrometer and a rotating copper anode x-ray source was used. The current and the voltage of the x-ray source were 150 mA and 50 kV, respectively, during operation. The anti-scattering slits and the anti-divergence slits were both set at 0.5°. The x-ray diffraction scan was carried out between 15° and 120° 2θ at a step size of 0.02° and the counting time per step was 0.6 seconds.

[0057] Samples S1, S2, S3 and S4, and Comparative Sample CS1, were tested in the Li coin cells described above, and the capacity fade after 50 cycles is provided in Table 2. The x-ray diffraction spectra were also obtained as described above. Their x and y values were calculated as described above with respect to the preferred embodiment of the invention and are also provided in Table 2.

[0058] In addition to the above samples, commercial samples C1, C2, C3 and C4 were also tested in the Li coin cells described above and their x-ray diffraction spectra were obtained the same way as samples S1, S2, S3, S4 and CS1. The capacity fade values after 50 cycles, as well as the x and y values are also provided for these commercial samples in Table 2.

	TABLE 2
				Capacity fade after
	samples	x	y	50 cycles
	S1	−3.22	−11.05	4%
	S2	−18.27	10.74	7%
	S3	14.55	−27.76	15%
	S4	−1.14	−14.71	4%
	CS1	21.53	−18.42	41%
	C1	14.46	−21.94	20%
	C2	8.86	−16.41	15%
	C3	11.91	−17.90	24%
	C4	28.51	−31.23	32%

[0059] FIG. 1 illustrates the positions of samples S1, S2, S3, and S4; comparative sample CS 1; and commercial samples C 1, C2, C3 and C4, in a principal component space as defined by the axes {right arrow over (P)}c1 and {right arrow over (P)}c2. The dotted line in FIG. 1 represents the equation x+0.77y=−6 in accordance with the preferred embodiment of the invention described above. As illustrated in FIG. 1, the samples prepared in accordance with the invention are on the left of the dotted line and the comparative and commercial samples are on the right of the dotted line.

[0060] FIG. 2 illustrates the capacity fade after 50 cycles versus x+0.77y. The dotted line in FIG. 2 defines the principal component space of the samples of the invention having the desired x-ray powder diffraction values and a fade of less than or equal to 15% in accordance with the preferred embodiment of the invention discussed above. In particular, the samples according to the invention S1, S2, S3 and S4 fall within in the principal component space (the box in the lower left portion of the graph) while the comparative sample and commercial examples do not. This demonstrates that the samples according to the invention have the capacity fade and the x-ray diffraction spectra that meet the equation xi+0.77 yi≦−6.

[0061] As shown above, the lithium cobalt oxides of the invention have good cycleability properties including good initial specific capacities and capacity fades and thus are desirable for use in rechargeable lithium and lithium-ion batteries. In addition, the lithium cobalt oxides of the present invention can be produced quickly in less than 10 hours and thus can be produced at a rate desired in the art.

[0062] It is understood that upon reading the above description of the present invention and studying the accompanying drawings, one skilled in the art could make changes and variations therefrom. These changes and variations are included in the spirit and scope of the following appended claims.

Claims

1. A method of preparing a lithium cobalt oxide LiwCo1−xAxO2+y having a hexagonal layered crystal structure wherein 0.96≦w≦1.05, 0≦x≦0.05,

2. The method according to claim 1, wherein said first heating step comprises heating the source compounds at a temperature of from about 500° C. to about 850° C.

3. The method according to claim 1, wherein said second heating step comprises heating the LiwCo1−xAxO2+y compound at a temperature from about 950° C. to about 980° C.

4. The method according to claim 1, wherein said first heating step comprises heating the source compounds at more than one firing temperature from about 500° C. to about 850° C.

5. The method according to claim 1, wherein said second heating step comprises heating the LiwCo1−xAxO2+y at more than one firing temperature from about 900° C. to about 1000° C.

6. The method according to claim 1, wherein said first heating step comprises heating the source compounds for a period of time of from about 30 minutes to about 3 hours.

7. The method according to claim 1, wherein said second heating step comprises heating the LiwCo1−xAxO2+y compound for a period of time of from about 30 minutes to about 7 hours.

8. The method according to claim 1, wherein said heating steps comprise heating the source compounds and the LiwCo1−xAxO2+y compound in a rotary calciner.

9. The method according to claim 1, wherein 0.98≦w≦1.02.

10. The method according to claim 1, wherein 0≦x≦0.02.

11. The method according to claim 1, wherein the lithium source compound is selected from the group consisting of Li2CO3 and LiOH and a cobalt source compound selected from the group consisting of Co3O4 and Co(OH)2.

12. The method according to claim 1, wherein said method further comprises the step of cooling the LiwCo1−xAxO2+y compound at a rate from 8° C./min to 140° C./min after said heating steps.

13. The method according to claim 1, wherein said method further comprises the step of cooling the LiwCo1−xAxO2+y compound at a rate from 10° C./min to 100° C./min after said heating steps.

14. The method according to claim 1, wherein the dopants A are one or more elements other than Co selected from the group consisting of Ni, Mn, Ti, Zr, V, Mo, Mg, Ca, Sr, Ba, Al, Ga, Si, Ge, Sn, and combinations thereof.

15. A lithium cobalt oxide prepared according to the method of claim 1.

16. A method of preparing a lithium cobalt oxide LiwCo1−xAxO2+y having a hexagonal layered crystal structure wherein 0.96≦w≦1.05, 0≦x≦0.05, −0.02≦y≦0.02 and A is one or more dopants other than Co selected from the group consisting of Ni, Mn, Ti, Zr, V, Mo, Mg, Ca, Sr, Ba, Al, Ga, Si, Ge, Sn, and combinations thereof, comprising the steps of: heating a lithium source compound, a cobalt source compound, and optionally one or more source compounds containing dopants A at a temperature from about 500° C. to about 850° C. for a period of time of from about 30 minutes to about 3 hours to produce LiwCo1−xAxO2+y; heating the LiwCo1−xAxO2+y compound at a temperature from about 900° C. to 1000° C. for a period of time of from about 30 minutes to about 7 hours to refine the hexagonal layered crystal structure; and cooling the LiwCo1−xAxO2+y compound at a rate from 8° C./min to 140° C./min after said heating steps.