Assessing Carrier Mobility, Dopability, and Defect Tolerance in the Chalcogenide Perovskite BaZrS_{3}

Abstract

The chalcogenide perovskite BaZrS_{3} 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 BaZrS_{3} has a phonon-limited electron mobility of 37cm^{2}/V s, which is comparable to that in halide perovskites, but lower hole mobility of 11cm^{2}/V s. The defect computations indicate that BaZrS_{3} 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 BaZrS_{3} 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 achieve longer carrier lifetime.