Atomic Model for Alkali Metal-Doped Tin–Lead Mixed Perovskites: Insight from Quantum Dynamics

Defects such as metal vacancies act as nonradiative recombination centers to deteriorate the photoelectric properties of metal halide perovskites. Nonadiabatic molecular dynamics has demonstrated that alkali metal dopants markedly improve the performance of mixed tin-lead perovskites. Alkali dopants increase the formation energy of tin vacancies to 1 eV, so that the defect concentration is decreased. When tin vacancies exist, alkali metals are easily doped into perovskites. Tin vacancies produce iodine trimers that create midgap states and cause rapid electron-hole recombination. Alkali metal additives eliminate the trap state, weaken nonadiabatic coupling, and decelerate charge recombination with a coefficient of ≤5.5 compared with the performance of the defective tin-lead mixed perovskite. Our research has constructed a theoretical model at the atomic level for alkali metal passivation that enhances defect tolerance of tin-lead mixed perovskites, generating valuable inspiration for optimizing high-performance perovskites.