Influence of Defects on Excited-State Dynamics in Lead Halide Perovskites: Time-Domain ab Initio Studies

This Perspective summarizes recent research into the excited-state dynamics in lead halide perovskites that are of paramount importance for photovoltaic and photocatalytic applications. Nonadiabatic molecular dynamics combined with time-domain ab initio density functional theory allows one to mimic time-resolved spectroscopy experiments at the atomistic level of detail. The focus is placed on realistic aspects of perovskite materials, including point defects, surfaces, grain boundaries, mixed stoichiometries, dopants, and interfaces. The atomistic description of the quantum dynamics of electron and hole trapping and recombination, provided by the time-domain ab initio simulations, generates important insights into the mechanisms of charge and energy losses and guides the development of high-performance perovskite solar cell devices.