Assessing Carrier Mobility, Dopability, and Defect Tolerance in the Chalcogenide Perovskite Ba Zr S 3

The chalcogenide perovskite Ba Zr S 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 Ba Zr S 3 has a phonon-limited electron mobility of 37 cm 2 / V s, which is comparable to that in halide perovskites, but lower hole mobility of 11 cm 2 / V s. The defect computations indicate that Ba Zr S 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 Ba Zr S 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.