Optical characterizations of the surface states in hybrid lead-halide perovskites

Methylammonium lead-iodide (CH 3 NH 3 PbI 3 , hereafter referred to as MAPbI 3 ) perovskite has emerged as a dazzling nova in the solar cell realm. To date, the surface physics of these materials is still puzzling, but in this work, we demonstrate that the optical dynamics in MAPbI 3 is primarily determined by the surface states. Pb dangling bonds on the surface of MAPbI 3 introduce shallow electronic states. The carrier localization effect for these electronic states is rather weak as the lifetimes of the carriers on the iodine-poor surface are comparative to those in the interior region of MAPbI 3 . In contrast, rich-iodine on the surface of MAPbI 3 induces deep trap centers for the carriers, which are detrimental to long carrier diffusion lengths. It is further proved that the surface passivation, which surprisingly prolongs the carrier diffusion lengths, mainly works on the rich-iodine on the surface rather than the Pb dangling bonds. This better understanding of the surface physics could provide essential information for improving the performance of photoelectronic devices based on MAPbI 3 perovskites. It is demonstrated that the optical dynamics in MAPbI 3 is primarily determined by the surface states. Pb dangling bonds in MAPbI 3 introduce shallow electronic states, whereas rich-iodine surface of MAPbI 3 induces deep trap centers for carriers which are detrimental to carrier lifetimes and diffusion lengths.