Protective Coating Interfaces for Perovskite Solar Cell Materials: A First-Principles Study

[Image: see text] The protection of halide perovskites is important for the performance and stability of emergent perovskite-based optoelectronic technologies. In this work, we investigate the potential inorganic protective coating materials ZnO, SrZrO(3), and ZrO(2) for the CsPbI(3) perovskite. The optimal interface registries are identified with Bayesian optimization. We then use semilocal density functional theory (DFT) to determine the atomic structure at the interfaces of each coating material with the clean CsI-terminated surface and three reconstructed surface models with added PbI(2) and CsI complexes. For the final structures, we explore the level alignment at the interface with hybrid DFT calculations. Our analysis of the level alignment at the coating–substrate interfaces reveals no detrimental mid-gap states but rather substrate-dependent valence and conduction band offsets. While ZnO and SrZrO(3) act as insulators on CsPbI(3), ZrO(2) might be suitable as an electron transport layer with the right interface engineering.