2025/02/27 by Andrew Grieder, Grieder, Andrew, Marcos F. Calegari Andrade +9
Engineering · Materials Science · Physics and Astronomy · #FOS: Physical sciences #Machine Learning in Materials Science #Materials Science (cond-mat.mtrl-sci) #Perovskite Materials and Applications #Strong Light-Matter Interactions
paper · pdf · doi:10.48550/arxiv.2502.20261
openalex publication_date 2025/02/27 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
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. 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.