Recent experiments report the rotation of FA (FA=HC[NH2]2+) cations significantly influence the excited-state lifetime of FAPbI3. However, the underlying mechanism remains unclear. Using ab initio nonadiabatic (NA) molecular dynamics combined with time-domain density functional simulations, we have demonstrated that reorientation of partial FA cations significantly inhibits nonradiative electron-hole recombination with respect to the pristine FAPbI3 due to the decreased NA coupling by localizing electron and hole in different positions and the suppressed atomic motions. Slow nuclear motions simultaneously increase the decoherence time, which is overcome by the reduced NA coupling, extending electron-hole recombination time scales to several nanoseconds and being about 3.9 times longer than that in pristine FAPbI3, which occurs within sub-nanosecond and agrees with experiment. Our study established the mechanism for the experimentally reported prolonged excited-state lifetime, providing a rational strategy for design of high performance of perovskite solar cells and optoelectronic devices.
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October 2020
Research Article|
October 01 2020
Charge localization induced by reorientation of FA cations greatly suppresses nonradiative electron-hole recombination in FAPbI3 perovskites: A time-domain Ab Initio study†
Jin-lu He;
Jin-lu He
College of Chemistry, Key Laboratory of Theoretical &
Computational Photochemistry of Ministry of Education, Beijing Normal
University
, Beijing 100875, China
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Yong-hao Zhu;
Yong-hao Zhu
College of Chemistry, Key Laboratory of Theoretical &
Computational Photochemistry of Ministry of Education, Beijing Normal
University
, Beijing 100875, China
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Run Long
Run Long
*
College of Chemistry, Key Laboratory of Theoretical &
Computational Photochemistry of Ministry of Education, Beijing Normal
University
, Beijing 100875, China
*Author to whom correspondence should be
addressed. E-mail: runlong@bnu.edu.cn
Search for other works by this author on:
*Author to whom correspondence should be
addressed. E-mail: runlong@bnu.edu.cn
†
Part of the special issue for “the Chinese Chemical Society’s 16th National Chemical Dynamics Symposium”.
Chin. J. Chem. Phys. 33, 642–648 (2020)
Article history
Received:
June 23 2020
Accepted:
July 24 2020
Citation
Jin-lu He, Yong-hao Zhu, Run Long; Charge localization induced by reorientation of FA cations greatly suppresses nonradiative electron-hole recombination in FAPbI3 perovskites: A time-domain Ab Initio study. Chin. J. Chem. Phys. 1 October 2020; 33 (5): 642–648. https://doi.org/10.1063/1674-0068/cjcp2006109
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