Unravelling the effects of oxidation state of interstitial iodine and oxygen passivation on charge trapping and recombination in CH3NH3PbI3 perovskite: a time-domain ab initio study.

ABSTRACT: Understanding nonradiative charge recombination mechanisms is a prerequisite for advancing perovskite solar cells. By performing time-domain density functional theory combined with nonadiabatic (NA) molecular dynamics simulations, we show that electron-hole recombination in perovskites strongly depends on the oxidation state of interstitial iodine and oxygen passivation. The simulations demonstrate that electron-hole recombination in CH3NH3PbI3 occurs within several nanoseconds, agreeing well with experiment. The negative interstitial iodine delays charge recombination by a factor of 1.3. The deceleration is attributed to the fact that interstitial iodine anion forms a chemical bond with its nearest lead atoms, eliminates the trap state, and decreases the NA electron-phonon coupling. The p

SUBMITTER: He J 

PROVIDER: S-EPMC6991187 | biostudies-literature | 2019 Nov

REPOSITORIES: biostudies-literature