Understanding structures and properties of phosphorene/perovskite heterojunction toward perovskite solar cell applications.

Two-dimensional black phosphorus (phosphorene) has drawn much attention in recent years due to its excellent electronic and optical properties. In this manuscript, we employ ab initio calculations to investigate the structural origin of the phosphorene/perovskite heterostructure. The calculations suggest that the chemical stability and the mechanical stability depend on the surface terminations, and the mechanical stability of the phosphorene/perovskite heterojunction should be further improved. The weak interactions between the P atoms in the phosphorene and the under-coordinated Pb atoms at the perovskite surfaces, as well as the weak interfacial charge transfer characters, are proposed to be mainly responsible for the moderate heterostructure stability. Suggestions to improve the stability of the heterojunction are provided. This study helps the fundamental understanding of the interaction between the phosphorene and the halide perovskite materials, and could provide a foundation for the better understanding of the low-dimensional materials in perovskite-based optoelectronic devices.