Abstract

Chalcogenide perovskites are gaining attention as strong candidates for replacing lead halide perovskites owing to their superior optoelectronic characteristics. Among these materials, BaZrS3 shows great promise as an absorber material for solar cells. However, with only limited available experimental data, there is a clear need for a deeper theoretical understanding to help guide future device development. In this study, we designed a BaZrS3-based solar cell and used SCAPS-1D simulations to compare the performance of delafossite hole-transport layers (CuFeO2, CuGaO2, and CuAlO2) with the commonly used Spiro-OMeTAD. We analyzed the impact of parameters like acceptor concentration, thickness of the active layer, and the absorber/HTL interface on device performance. Our findings indicate that optimizing the acceptor concentration significantly improves VOC across all HTLs by enhancing the quasi-Fermi level splitting and strengthening the internal electrostatic field. Enhancing the thickness of the active layer to 800 nm improves photon absorption, boosting about 31 %, resulting in increased charge carrier generation. However, introducing more defects in the absorber drastically reduces the power conversion efficiency (PCE) to approximately 0.09 % owing to greater recombination losses. After optimization, the devices using CuFeO2, CuGaO2, CuAlO2, and Spiro-OMeTAD achieved PCEs of 28.34 %, 27.83 %, 25.04 %, and 27.80 %, respectively. These improvements are mainly due to the higher built-in potential, stronger light absorption, and better charge-carrier dynamics. Overall, this study offers useful theoretical insights to support the development of efficient BaZrS3-based chalcogenide perovskite solar cells. © 2025 Elsevier B.V.