Low-frequency lattice phonons in halide perovskites explain high defect tolerance toward electron-hole recombination

Chu, Weibin; Zheng, Qijing; Prezhdo, Oleg V.; Zhao, Jin; Saidi, Wissam A.

doi:10.1126/sciadv.aaw7453

Low-frequency lattice phonons in halide perovskites explain high defect tolerance toward electron-hole recombination

Journal Article · Fri Jan 31 23:00:00 EST 2020 · Science Advances

DOI:https://doi.org/10.1126/sciadv.aaw7453· OSTI ID:1626015

^[1]; ^[2]; Prezhdo, Oleg V. ^[3]; ^[4]; ^[5]

University of Science and Technology of China, Hefei (China). ICQD/Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics; Univ. of Southern California, Los Angeles, CA (United States). Departments of Chemistry, and Physics and Astronomy; DOE/OSTI
University of Science and Technology of China, Hefei (China). ICQD/Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics
Univ. of Southern California, Los Angeles, CA (United States). Departments of Chemistry, and Physics and Astronomy
University of Science and Technology of China, Hefei (China). ICQD/Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics; Univ. of Pittsburgh, PA (United States). Department of Physics and Astronomy; University of Science and Technology of China, Hefei (China).Synergetic Innovation Center of Quantum Information and Quantum Physics
niv. of Pittsburgh, PA (United States). Department of Mechanical Engineering and Materials Science

Low-cost solution-based synthesis of metal halide perovskites (MHPs) invariably introduces defects in the system, which could form Shockley-Read-Hall (SRH) electron-hole recombination centers detrimental to solar conversion efficiency. Here, we investigate the nonradiative recombination processes due to native point defects in methylammonium lead halide (MAPbI₃) perovskites using ab initio nonadiabatic molecular dynamics within surface-hopping framework. Regardless of whether the defects introduce a shallow or deep band state, we find that charge recombination in MAPbI₃is not enhanced, contrary to predictions from SRH theory. We demonstrate that this strong tolerance against defects, and hence the breakdown of SRH, arises because the photogenerated carriers are only coupled with low-frequency phonons and electron and hole states overlap weakly. Both factors appreciably decrease the nonadiabatic coupling. We argue that the soft nature of the inorganic lattice with small bulk modulus is key for defect tolerance, and hence, the findings are general to other MHPs.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Southern California, Los Angeles, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357; SC0014429

OSTI ID:: 1626015

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 7 Vol. 6; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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