Coupled Electronic and Anharmonic Structural Dynamics for Carrier Self-Trapping in Photovoltaic Antimony Chalcogenides

doi:10.1002/advs.202202154

	Coupled Electronic and Anharmonic Structural Dynamics for Carrier Self-Trapping in Photovoltaic Antimony Chalcogenides
	Tao, Weijian 1; Zhu, Leilei 2; Li, Kanghua 3,4; Chen, Chao 3,4; Chen, Yuzhong 1; Li, Yujie 1; Li, Xufeng 1; Tang, Jiang 3,4; Shang, Honghui 2; Zhu, Haiming 1,5
	2022-06-26
发表期刊	ADVANCED SCIENCE
页码	9
摘要	V-VI antimony chalcogenide semiconductors have shown exciting potentials for thin film photovoltaic applications. However, their solar cell efficiencies are strongly hampered by anomalously large voltage loss (>0.6 V), whose origin remains controversial so far Herein, by combining ultrafast pump-probe spectroscopy and density functional theory (DFT) calculation, the coupled electronic and structural dynamics leading to excited state self-trapping in antimony chalcogenides with atomic level characterizations is reported. The electronic dynamics in Sb2Se3 indicates a approximate to 20 ps barrierless intrinsic self-trapping, with electron localization and accompanied lattice distortion given by DFT calculations. Furthermore, impulsive vibrational coherences unveil key Sb-Se vibrational modes and their real-time interplay that drive initial excited state relaxation and energy dissipation toward stabilized small polaron through electron-phonon and subsequent phonon-phonon coupling. This study's findings provide conclusive evidence of carrier self-trapping arising from intrinsic lattice anharmonicity and polaronic effect in antimony chalcogenides and a new understanding on the coupled electronic and structural dynamics for redefining excited state properties in soft semiconductor materials.
关键词	antimony chalcogenides carrier self-trapping electron-phonon interaction
DOI	10.1002/advs.202202154
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China[22022305] ; National Natural Science Foundation of China[22003073] ; National Natural Science Foundation of China[61904058] ; National Natural Science Foundation of China[61725401] ; National Natural Science Foundation of China[62174064] ; National Key Research and Development Program of China[2017YFA0207700] ; National Key Research and Development Program of China[2016YFA0200604] ; National Key Research and Development Program of China[2017YFA0204904]
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science
WOS类目	Chemistry, Multidisciplinary ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS记录号	WOS:000815786000001
出版者	WILEY
引用统计	被引频次：21[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://119.78.100.204/handle/2XEOYT63/19535
专题	中国科学院计算技术研究所期刊论文_英文
通讯作者	Shang, Honghui; Zhu, Haiming
作者单位	1.Zhejiang Univ, Dept Chem, State Key Lab Modern Opt Instrumentat, Key Lab Excited State Mat Zhejiang Prov, Hangzhou 310027, Zhejiang, Peoples R China 2.Chinese Acad Sci, Inst Comp Technol, State Key Lab Comp Architecture, Beijing 100190, Peoples R China 3.Huazhong Univ Sci & Technol, Wuhan Natl Lab Optoelect, Wuhan 430074, Hubei, Peoples R China 4.Huazhong Univ Sci & Technol, Sch Opt & Elect Informat, Wuhan 430074, Hubei, Peoples R China 5.Zhejiang Univ Hangzhou Global Sci & Technol Innov, Hangzhou 310014, Peoples R China
推荐引用方式 GB/T 7714	Tao, Weijian,Zhu, Leilei,Li, Kanghua,et al. Coupled Electronic and Anharmonic Structural Dynamics for Carrier Self-Trapping in Photovoltaic Antimony Chalcogenides[J]. ADVANCED SCIENCE,2022:9.
APA	Tao, Weijian.,Zhu, Leilei.,Li, Kanghua.,Chen, Chao.,Chen, Yuzhong.,...&Zhu, Haiming.(2022).Coupled Electronic and Anharmonic Structural Dynamics for Carrier Self-Trapping in Photovoltaic Antimony Chalcogenides.ADVANCED SCIENCE,9.
MLA	Tao, Weijian,et al."Coupled Electronic and Anharmonic Structural Dynamics for Carrier Self-Trapping in Photovoltaic Antimony Chalcogenides".ADVANCED SCIENCE (2022):9.