Asynchronous Photoexcited Electronic and Structural Relaxation in Lead-Free Perovskites

doi:10.1021/jacs.9b04557

	Asynchronous Photoexcited Electronic and Structural Relaxation in Lead-Free Perovskites
	Liu, Cunming 1; Wang, Yingqi 3; Geng, Huifang 4; Zhu, Taishan 5; Ertekin, Elif 5; Gosztola, David 2; Yang, Sizhuo 6; Huang, Jier 6; Yang, Bin 7; Han, Keli 7
刊名	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
	2019-08-21
卷号	141 期号:33 页码:13074-13080
ISSN号	0002-7863
DOI	10.1021/jacs.9b04557
通讯作者	Zheng, Kaibo(kaibo.zheng@chemphys.lu.se) ; Zhang, Xiaoyi(xyzhang@aps.anl.gov)
英文摘要	Vacancy-ordered lead-free perovskites with more-stable crystalline structures have been intensively explored as the alternatives for resolving the toxic and long-term stability issues of lead halide perovskites (LHPs). The dispersive energy bands produced by the closely packed halide octahedral sublattice in these perovskites are meanwhile anticipated to facility the mobility of charge carriers. However, these perovskites suffer from unexpectedly poor charge carrier transport. To tackle this issue, we have employed the ultrafast, elemental-specific X-ray transient absorption (XTA) spectroscopy to directly probe the photoexcited electronic and structural dynamics of a prototypical vacancy-ordered lead-free perovskite (Cs3Bi2Br9). We have discovered that the photogenerated holes quickly self-trapped at Br centers, simultaneously distorting the local lattice structure, likely forming small polarons in the configuration of V-k center (Br-2(-) dimer). More significantly, we have found a surprisingly long-lived, structural distorted state with a lifetime of, similar to 59 mu s, which is similar to 3 orders of magnitude slower than that of the charge carrier recombination. Such long-lived structural distortion may produce a transient "background" under continuous light illumination, influencing the charge carrier transport along the lattice framework.
资助项目	U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences[DE-AC02-06CH11357] ; China Scholarship Council ; Helmholtz Recognition Award ; European Union[GINOP-2.3.6-15-2015-00001] ; European Regional Development Fund[GINOP-2.3.6-15-2015-00001] ; NSF[PIRE 1545907] ; NSF Career Award (DMR)[1654140] ; National Natural Science Foundation of China[21533010] ; Danish Council for Independent Research[7026-0037B] ; Swedish Research Council[2017-05337] ; New Facility and Midscale Instrumentation grants ; DOE Office of Science[DE-AC02-06CH11357]
WOS关键词	HALIDE PEROVSKITE ; EFFICIENT ; SEMICONDUCTORS ; POLARONS ; STATE ; HOLE
WOS研究方向	Chemistry
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000482546400023
资助机构	U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences ; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences ; China Scholarship Council ; China Scholarship Council ; Helmholtz Recognition Award ; Helmholtz Recognition Award ; European Union ; European Union ; European Regional Development Fund ; European Regional Development Fund ; NSF ; NSF ; NSF Career Award (DMR) ; NSF Career Award (DMR) ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Danish Council for Independent Research ; Danish Council for Independent Research ; Swedish Research Council ; Swedish Research Council ; New Facility and Midscale Instrumentation grants ; New Facility and Midscale Instrumentation grants ; DOE Office of Science ; DOE Office of Science ; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences ; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences ; China Scholarship Council ; China Scholarship Council ; Helmholtz Recognition Award ; Helmholtz Recognition Award ; European Union ; European Union ; European Regional Development Fund ; European Regional Development Fund ; NSF ; NSF ; NSF Career Award (DMR) ; NSF Career Award (DMR) ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Danish Council for Independent Research ; Danish Council for Independent Research ; Swedish Research Council ; Swedish Research Council ; New Facility and Midscale Instrumentation grants ; New Facility and Midscale Instrumentation grants ; DOE Office of Science ; DOE Office of Science ; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences ; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences ; China Scholarship Council ; China Scholarship Council ; Helmholtz Recognition Award ; Helmholtz Recognition Award ; European Union ; European Union ; European Regional Development Fund ; European Regional Development Fund ; NSF ; NSF ; NSF Career Award (DMR) ; NSF Career Award (DMR) ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Danish Council for Independent Research ; Danish Council for Independent Research ; Swedish Research Council ; Swedish Research Council ; New Facility and Midscale Instrumentation grants ; New Facility and Midscale Instrumentation grants ; DOE Office of Science ; DOE Office of Science ; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences ; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences ; China Scholarship Council ; China Scholarship Council ; Helmholtz Recognition Award ; Helmholtz Recognition Award ; European Union ; European Union ; European Regional Development Fund ; European Regional Development Fund ; NSF ; NSF ; NSF Career Award (DMR) ; NSF Career Award (DMR) ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Danish Council for Independent Research ; Danish Council for Independent Research ; Swedish Research Council ; Swedish Research Council ; New Facility and Midscale Instrumentation grants ; New Facility and Midscale Instrumentation grants ; DOE Office of Science ; DOE Office of Science
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/173275]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Zheng, Kaibo; Zhang, Xiaoyi
作者单位	1.Argonne Natl Lab, Xray Sci Div, 9700 S Cass Ave, Lemont, IL 60439 USA 2.Argonne Natl Lab, Ctr Nanoscale Mat, 9700 S Cass Ave, Lemont, IL 60439 USA 3.Ctr High Pressure Sci & Technol Adv Res, Shanghai 201203, Peoples R China 4.ELI HU Nonprofit Ltd, ELI ALPS, Dugonics Ter 13, H-6720 Szeged, Hungary 5.Univ Illinois, Dept Mech Sci & Engn, 1206 West Green St, Urbana, IL 61801 USA 6.Marquette Univ, Dept Chem, Milwaukee, WI 53201 USA 7.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian, Peoples R China 8.DESY, Notkestr 85, D-22607 Hamburg, Germany 9.Sychrotron Soleil, F-91192 Gif Sur Yvette, France 10.Lund Univ, Dept Chem Phys & Nanolund, Box 124, S-22100 Lund, Sweden
推荐引用方式 GB/T 7714	Liu, Cunming,Wang, Yingqi,Geng, Huifang,et al. Asynchronous Photoexcited Electronic and Structural Relaxation in Lead-Free Perovskites[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2019,141(33):13074-13080.
APA	Liu, Cunming.,Wang, Yingqi.,Geng, Huifang.,Zhu, Taishan.,Ertekin, Elif.,...&Zhang, Xiaoyi.(2019).Asynchronous Photoexcited Electronic and Structural Relaxation in Lead-Free Perovskites.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,141(33),13074-13080.
MLA	Liu, Cunming,et al."Asynchronous Photoexcited Electronic and Structural Relaxation in Lead-Free Perovskites".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 141.33(2019):13074-13080.