Ultrafast Charge Transfer at CH₃NH₃PbI₃ and MoS₂ Interface

To achieve higher power conversion efficiency of promising hybrid organic-inorganic perovskites (HOIP), interface engineering must be applied to optimize the charge carrier pathway from absorber to electron and hole transport layers. Fast charge transfer can largely avoid charge accumulation at the interface, and suppress recombination. Further, optimized band alignment between charge transfer material and adsorber would reduce the “potential loss” in the conversion efficiency of the solar cell. Herein, we employ nonadiabatic molecular dynamics (NAMD) within time dependent density functional theory to study hole transfer from CH₃NH₃PbI₃ to monolayer MoS₂. Our results show that there is an ultrafast hole transfer channel in agreement with a recent experimental study. Because of the existence of a fast charge transfer and minimal band mismatch between CH₃NH₃PbI₃ and MoS₂ at the same time, MoS₂ is a promising hole transfer material in HOIP.