Lattice Distortion and Low-Frequency Anharmonic Phonons Suppress Charge Recombination in Lead Halide Perovskites upon Pseudohalide Doping: Time-Domain Ab Initio Analysis

被引:5
作者
Lu, Teng-Fei [1 ]
Chu, Weibin [2 ]
Agrawal, Sraddha [3 ]
Zhang, Zhihua [1 ]
Prezhdo, Oleg V. [3 ]
机构
[1] Dalian Jiaotong Univ, Sch Mat Sci & Engn, Dalian 116028, Liaoning, Peoples R China
[2] Fudan Univ, Inst Computat Phys Sci, Key Lab Computat Phys Sci, Minist Educ, Shanghai 200433, Peoples R China
[3] Univ Southern Calif, Dept Chem, Los Angeles, CA 90089 USA
关键词
ELECTRON-HOLE RECOMBINATION; MOLECULAR-DYNAMICS; PYXAID PROGRAM; PERFORMANCE;
D O I
10.1021/acs.jpclett.3c02850
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Perovskite solar cells have witnessed a surge in interest as a promising technology for low-cost, high-efficiency photovoltaics with certified power conversion efficiencies beyond 25%. However, their commercial development is hindered by poor stability and nonradiative losses that restrict their approach to the theoretical efficiency limit. Using ab initio nonadiabatic molecular dynamics, we demonstrate that nonradiative charge recombination is suppressed when the iodide in formamidinium lead iodide (FAPbI(3)) is partially replaced with pseudohalide anions (SCN-, BF4 -, and PF6 (-)). The replacement breaks the symmetry of the system and creates local structural distortion and dynamic disorder, decreasing electron-hole overlap and nonadiabatic electron-vibrational coupling. The charge carrier lifetime is found to increase with increased structural distortion and is the longest for PF6 -. This work is fundamentally relevant to the design of high-performance perovskite materials for optoelectronic applications.
引用
收藏
页码:10685 / 10692
页数:8
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