Carrier Localization in Pnictogen-Based Chalcohalides from Defect-Bound Hot Polarons
Abstract
Pnictogen-based solar absorbers have gained prominence as promising nontoxic and stable alternatives to lead-halide perovskites (LHPs), but are severely limited by carrier localization, preventing their performance from approaching those of LHPs. Recent efforts have uncovered routes to overcome carrier localization, but these early efforts only considered intrinsic factors. Herein, we push beyond these limited early efforts, examining the role of defects, not only on cold carriers but also hot carriers. Focusing on the structurally one-dimensional pnictogen chalcohalide BiSBr, we find that whilst this material intrinsically does not exhibit carrier localization, vacancies introduced during synthesis or post-treatment lead to pronounced extrinsic self-trapping via the formation of defect-bound hot polarons-excited charge-carriers strongly coupled to local defect-induced vibrational modes. These above-gap defect states divert hot carriers from cooling to the band edge, thus depleting the mobile carrier population. Our findings establish the key role of defect-bound hot polarons in mediating extrinsic localization and offer new mechanistic insights into the interplay between defects, lattice coupling, and excited-state charge-carrier transport, which are critical to designing efficient perovskite-inspired solar absorbers.
Comments: 20 pages, 5 figures
Cite
@article{arxiv.2605.29925,
title = {Carrier Localization in Pnictogen-Based Chalcohalides from Defect-Bound Hot Polarons},
author = {Xiaoyu Guo and Junzhi Ye and Cibrán Lopez Alvarez and Maciej Oskar Liedke and Maik Butterling and Mutibah Alanazi and Yi-Teng Huang and Jiajie Wu and Zhilong Zhang and Lars Van Turnhout and Yorrick Boeije and Bofeng Xue and Qingyu Wang and Hugh Lohan and Seán R. Kavanagh and Andreas Wagner and Eric Hirschmann and Robert A. Taylor and Akshay Rao and Edgardo Saucedo and Claudio Cazorla and Robert L. Z. Hoye},
journal= {arXiv preprint arXiv:2605.29925},
year = {2026}
}