A-site Cation Effects on Hot Carrier Relaxation in Perovskites by Nonadiabatic Molecular Dynamics Simulations †

doi:10.7503/cjcu20190701

Abstract

Abstract:

In recent years, perovskites have become a research hotspot in the field of solar cells due to their excellent optical and electrical properties. A large number of experiments reported that hot carries relaxation times follow the trend CsPbBr₃>MAPbBr₃(MA=CH₃NH₃)>FAPbBr₃[FA=HC(NH₂)₂]. However, the underlying mechanism of the A-site cation(Cs ⁺, MA ⁺, FA ⁺) effects on the relaxation time remains unclear, the hot electrons and holes relaxation of the three perovskiteswere investigated using time-domain density functional theory combined with nonadiabatic molecular dynamics. The obtained time scales agreed well with experiment. This is because A-site cation affects electronic-vibrational coupling with the inorganic Pb—Br framework via electrostatic interaction and hydrogen bond, leading to the strength of nonadiabatic coupling decreasing from FAPbBr₃ to MAPbBr₃, to CsPbBr₃. As a result, the hot carrier relaxation times decreases as the same trend. The study suggests that rational choice of A-site cations provides an excellent strategy to the optimize the performance of perovskite solar cells.

Key words: Perovskite, A-site cation, Hot carrier energy relaxation, Nonadiabatic molecular dynamics, Time-dependent density functional theory

CLC Number:

O641

TrendMD:

HE Jinlu, LONG Run, FANG Weihai. A-site Cation Effects on Hot Carrier Relaxation in Perovskites by Nonadiabatic Molecular Dynamics Simulations ^†[J]. Chem. J. Chinese Universities, 2020, 41(3): 439.

Figures/Tables 5

Fig.1 Schematic diagram of hot carrier energy relaxation dynamics in the perovskite system

Fig.2 Simulation cell showing the optimized geometry and a representative snapshot of molecular dynamics at 300 K of CsPbBr3, MAPbBr3 and FAPbBr3

Fig.3 Projected density of states(PDOS) of CsPbBr3(A), MAPbBr3(B) and FAPbBr3(C) systems

Fig.4 Time evolution of the energy decay dynamics of hot electrons with 0.4 eV(A)and 0.6 eV(C) excess energies, and hot holes with 0.4 eV(B) and 0.6 eV(D) excess energies

Fig.5 Average magnitude of the nonadiabatic couplings for hot electrons and holes relaxation within conduction band and valence band of the CsPbBr3, MAPbBr3 and FAPbBr3

References 54

[1]	De Wolf S., Holovsky J., Moon S. J., Löper P., Niesen B., Ledinsky M., Haug F. J., Yum J. H., Ballif C ., J. Phys. Chem. Lett., 2014, 5, 1035— 1039
[2]	Shi D., Adinolfi V., Comin R., Yuan M., Alarousu E., Buin A., Chen Y., Hoogland S., Rothenberger A., Katsiev K ., Science, 2015, 347, 519— 522
[3]	Zhu H., Miyata K., Fu Y., Wang J., Joshi P. P., Niesner D., Williams K. W., Jin S., Zhu X. Y ., Science, 2016, 353, 1409— 1413
[4]	Zhu H., Fu Y., Meng F., Wu X., Gong Z., Ding Q., Gustafsson M. V., Trinh M. T., Jin S., Zhu X. Y ., Nature Materials, 2015, 14, 636— 642
[5]	Wang J., Dong J., Lu F., Sun C., Zhang Q., Wang N ., J. Mater. Chem. A, 2019, 7, 23563— 23576
[6]	Azpiroz J. M., Mosconi E., Bisquert J., de Angelis F ., Energy Environ. Sci., 2015, 8, 2118—2127
[7]	Dong X., Fang X., Lü M. H., Lin B. C., Zhang S., Wang Y., Yuan N. Y., Ding J. N ., Chinese Science Bulletin, 2016,1025
	( 董旭, 房香, 吕明航, 林本才, 张帅, 王莹, 袁宁一, 丁建宁 . 科学通报, 2016,1025)
[8]	Chen C., Yang X. C., Liu W., ., CIESC J., 2017, 811— 820
	( 陈超, 杨修春, 刘巍 . 化工学报, 2017, 811— 820)
[9]	Gan Y. S., Chen M. M., Wang Y. L., Wan L., Kong M. Q., Hu H., Wang S. M ., Materials Reports, 2018, 32, 4047—4050, 4078
	( 甘一升, 陈苗苗, 王玉龙, 万丽, 孔梦琴, 胡航, 王世敏 . 材料导报, 2018, 32, 4047—4050, 4078)
[10]	Zhang D. F., Zheng L. L., Ma Y. Z., Wang S. F., Bian Z. Q., Huang C. H., Gong Q. H., Xiao L. X ., Acta Physica Sinica, 2015, 64, 118— 124
	( 张丹霏, 郑灵灵, 马英壮, 王树峰, 卞祖强, 黄春辉, 龚旗煌, 肖立新 . 物理学报, 2015, 64, 118— 124)
[11]	Kojima A., Teshima K., Shirai Y., Miyasaka T ., J. Am. Chem. Soc., 2009, 131, 6050— 6051
[12]	NREL, Efficiency Chart., 2019,
[13]	Rühle S ., Sol. Energy, 2016, 130, 139— 147
[14]	Jeon N. J., Noh J. H., Yang W. S., Kim Y. C., Ryu S., Seo J., Seok S. I ., Nature, 2015, 517, 476— 480
[15]	Fu J., Xu Q., Han G., Wu B., Huan C. H. A., Leek M. L., Sum T. C ., Nat. Commun., 2017, 8, 1300
[16]	Chung H., Jung S. I., Kim H. J., Cha W., Sim E., Kim D., Koh W. K., Kim J ., Angew. Chem. Int. Ed. Engl., 2017, 56, 4160— 4164
[17]	Chen J., Messing M. E., Zheng K., Pullerits T ., J. Am. Chem. Soc., 2019, 141, 3532— 3540
[18]	Fang H. H., Adjokatse S., Shao S., Even J., Loi M. A ., Nat. Commun., 2018, 9, 243
[19]	Wang Y., Long R ., J. Phys. Chem. Lett., 2019, 10, 4354— 4361
[20]	Qiao L., Sun X., Long R ., J. Phys. Chem. Lett., 2019, 10, 672— 678
[21]	He J., Fang W. H., Long R., Prezhdo O. V ., ACS Energy Lett., 2018, 3,2070—2076
[22]	Hopper T. R., Gorodetsky A., Frost J. M., Müller C., Lovrincic R., Bakulin A. A ., ACS Energy Lett., 2018, 3, 2199— 2205
[23]	Petersilka M., Gossmann U., Gross E ., Phys. Rev. Lett., 1996, 76, 1212— 1215
[24]	Tully J. C ., J. Chem. Phys., 1990, 93, 1061— 1071
[25]	Craig C. F., Duncan W. R., Prezhdo O. V ., Phys. Rev. Lett., 2005, 95, 163001
[26]	Fischer S. A., Habenicht B. F., Madrid A. B., Duncan W. R., Prezhdo O. V ., J. Chem. Phys., 2011, 134, 024102
[27]	Kohn W., Sham L. J ., Phys. Rev., 1965, 140, A1133— A1138
[28]	Isborn C. M., Li X., Tully J. C ., J. Chem. Phys., 2007, 126, 134307
[29]	Hammes-Schiffer S., Tully J. C ., J. Chem. Phys., 1994, 101, 4657— 4667
[30]	Parandekar P. V., Tully J. C ., J. Chem. Phys., 2005, 122, 094102
[31]	Fabiano E., Keal T., Thiel W ., Chem. Phys., 2008, 349, 334— 347
[32]	Kapral R., Ciccotti G ., J. Chem. Phys., 1999, 110, 8919— 8929
[33]	Herman M. F., Kluk E ., Chem. Phys., 1984, 91, 27— 34
[34]	Tully J ., Faraday Discuss., 1998, 110, 407— 419
[35]	Akimov A. V., Prezhdo O. V ., J. Chem. Theory Comput., 2013, 9, 4959— 4972
[36]	Wang S., Luo Q., Fang W. H., Long R ., J. Phys. Chem. Lett., 2019, 10, 1234— 1241
[37]	Long R., Prezhdo O. V ., Nano Lett., 2014, 14, 3335— 3341
[38]	Li W., Sun Y. Y., Li L., Zhou Z., Tang J., Prezhdo O. V ., J. Am. Chem. Soc., 2018, 140, 15753— 15763
[39]	Long R., Prezhdo O. V ., Nano Lett., 2015, 15, 4274— 4281
[40]	Kresse G., Furthmüller J ., Phys. Rev. B, 1996, 54, 11169— 11186
[41]	Perdew J. P., Burke K., Ernzerhof M ., Phys. Rev. Lett., 1996, 77, 3865— 3868
[42]	Blöchl P. E ., Phys. Rev. B, 1994, 50, 17953— 17979
[43]	Monkhorst H. J., Pack J. D ., Phys. Rev. B, 1976, 13, 5188— 5192
[44]	Grimme S., Antony J., Ehrlich S., Krieg H ., J. Chem. Phys., 2010, 132, 154104
[45]	Rodová M., Brožek J., Knížek K., Nitsch K ., J. Therm. Anal. Calorim., 2003, 71, 667— 673
[46]	Elbaz G. A., Straus D. B., Semonin O. E., Hull T. D., Paley D. W., Kim P., Owen J. S., Kagan C. R., Roy X ., Nano Lett., 2017, 17, 1727— 1732
[47]	Zhumekenov A. A., Saidaminov M. I., Haque M. A., Alarousu E., Sarmah S. P., Murali B., Dursun I., Miao X. H., Abdelhady A. L., Wu T ., ACS Energy Lett., 2016, 1, 32— 37
[48]	Knop O. W., Wasylishen R. E., White M. A., Cameron T. S., Oort M. J. V ., Can. J. Chem., 1990, 68, 412— 422
[49]	Sun S., Isikgor F. H., Deng Z., Wei F., Kieslich G., Bristowe P. D., Ouyang J., Cheetham A. K ., ChemSusChem, 2017, 10, 3740— 3745
[50]	Jankowska J., Prezhdo O. V ., J. Phys. Chem. Lett., 2017, 8, 812— 818
[51]	Motta C., El-Mellouhi F., Sanvito S ., Phys. Rev. B, 2016, 93, 235412
[52]	El-Mellouhi F., Marzouk A., Bentria E. T., Rashkeev S. N., Kais S., Alharbi F. H ., ChemSusChem, 2016, 9, 2648— 2655
[53]	Ye Y., Run X., Xu H. T., Feng H., Fei X., Wang L. J ., Chin. Phys. B, 2015, 24, 116302— 116303
[54]	Tavernelli I., Tapavicza E., Rothlisberger U ., J. Chem. Phys., 2009, 130, 124107

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