English

Distinguishing thermal fluctuations from polaron formation in halide perovskites

Materials Science 2025-02-13 v2

Abstract

Recent angle-resolved photoelectron spectroscopy (ARPES) measurements of the hole effective mass in CsPbBr3_3 revealed an enhancement of \sim50 % compared to the bare mass computed from first principles for CsPbBr3_3 at T=0KT = 0 K. This large enhancement was interpreted as evidence of polaron formation. Employing accurate finite-temperature first-principles calculations, we show that the calculated hole effective mass of CsPbBr3_3 at T=300KT = 300 K can explain experimental results without invoking polarons. Thermal fluctuations are particularly strong in halide perovskites compared to conventional semiconductors such as Si and GaAs, and cannot be ignored when comparing with experiment. We not only resolve the debate on polaron formation in halide perovskites, but also demonstrate the general importance of including thermal fluctuations in first-principles calculations for strongly anharmonic materials.

Keywords

Cite

@article{arxiv.2502.06904,
  title  = {Distinguishing thermal fluctuations from polaron formation in halide perovskites},
  author = {Bai-Qing Zhao and Xuan-Yan Chen and Chuan-Nan Li and Jinshan Li and Chris G. Van de Walle and Xie Zhang},
  journal= {arXiv preprint arXiv:2502.06904},
  year   = {2025}
}