Carrier Localization and Spontaneous Formation of Two-Dimensional Polarization Domain in Halide Perovskites

Grieder, Andrew; Andrade, Marcos Calegari; Takenaka, Hiroyuki; Ogitsu, Tadashi; Tan, Liang Z.; Ping, Yuan

doi:10.1103/4kyt-jj6w

Carrier Localization and Spontaneous Formation of Two-Dimensional Polarization Domain in Halide Perovskites

Journal Article · Wed Sep 24 00:00:00 EDT 2025 · Physical Review Letters

DOI:https://doi.org/10.1103/4kyt-jj6w· OSTI ID:2589921

^[1]; ^[2]; Takenaka, Hiroyuki ^[3]; ^[4]; ^[5]; ^[1]

Univ. of Wisconsin, Madison, WI (United States)
Univ. of California, Santa Cruz, CA (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Univ. of California, Santa Cruz, CA (United States)
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry

Halide perovskites are known for their rich phase diagram and superior performance in diverse optoelectronics applications. The latter property is often attributed to the long electron-hole recombination time, whose underlying physical mechanism has been a long-standing controversy. In this Letter, we investigate the transport and localization properties of electron and hole carriers in a prototypical halide perovskite (CsPbBr₃), through ab initio tight-binding nonadiabatic dynamics approach for large-scale (tens of nm size) supercell calculations, to simulate electron and ion dynamics on the same footing. Here, we found distinct structural, lattice polarization, and electron-phonon coupling properties at low (below 100 K) and high temperatures, consistent with experimental observations. In particular, at low temperature we find spontaneous formation of polar grain boundaries in the nonpolar bulk systems, which result in two-dimensional polarization patterns that serve to localize and separate electrons and holes. We reveal phonon-assisted variable-range hopping mostly responsible for low-temperature transport, and their characteristic frequency correlates with temperature-dependent phonon power spectrum and energy oscillation frequency in nonadiabatic dynamics. We answer the critical questions of long electron-hole recombination lifetime at low temperature and offer the correlation among polarization domains, electron-phonon couplings, and photocarrier dynamics.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: National Energy Research Scientific Computing Center (NERSC); National Science Foundation (NSF); USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231; AC52-07NA27344; SC0023301

Other Award/Contract Number:: CHE-2203633
BES-ERCAP0032784

OSTI ID:: 2589921

Alternate ID(s):: OSTI ID: 3021982

Report Number(s):: LLNL--JRNL-2011902; ark:/13030/qt3jp5v7dt; https://escholarship.org/uc/item/3jp5v7dt

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 13 Vol. 135; ISSN 1079-7114; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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