The chalcogenide perovskite BaZrS3 has attracted much attention as a promising solar absorber for thin-film photovoltaics. Here, we use first-principles calculations to evaluate its carrier transport and defect properties. We find that BaZrS3 has a phonon-limited electron mobility of 37 cm2/Vs comparable to that in halide perovskites but lower hole mobility of 11 cm2/Vs. The defect computations indicate that BaZrS3 is intrinsically n-type due to shallow sulfur vacancies, but that strong compensation by sulfur vacancies will prevent attempts to make it p-type. We also establish that BaZrS3 shows some degree of defect tolerance, presenting only few low formation energy, deep intrinsic defects. Among the deep defects, sulfur interstitials are the dominant nonradiative recombination centers but exhibit a moderate capture coefficient. Our work highlights the material's intrinsic limitations in carrier mobility and p-type doping and suggests focusing on suppressing the formation of sulfur interstitials to reach longer carrier lifetime.
@article{arxiv.2405.09793,
title = {Assessing carrier mobility, dopability, and defect tolerance in the chalcogenide perovskite BaZrS$_3$},
author = {Zhenkun Yuan and Diana Dahliah and Romain Claes and Andrew Pike and David P. Fenning and Gian-Marco Rignanese and Geoffroy Hautier},
journal= {arXiv preprint arXiv:2405.09793},
year = {2024}
}