Excited-State Dynamics in Metal Halide Perovskites: A Theoretical Perspective

The chapter summarizes recent research activities in the atomistic modeling of photoexcitation dynamics relevant to metal halide perovskite (MHP) solar cells and other optoelectronic applications. The influence of realistic aspects of material composition and structure on nonradiative relaxation of charge carriers, hot-carrier cooling and trapping, and interfacial charge separation and recombination are illustrated using representative materials and interfaces. Focus is placed on point defects, mixed stoichiometries, dopants, surfaces and their passivation, grain boundaries, and interfaces of MHPs with charge transport layers. In addition to bulk materials, two-dimensional perovskites with different layer and spacer structures, edge passivations, and dielectric screening are discussed. Advanced physical phenomena, such as ferroelectric ordering, hot charge carriers, hot luminescence, quantum confinement, multiple excitons, and synergy between different dynamic processes, are considered. The atomistic description of the quantum dynamics under realistic conditions guides the development of high-performance perovskite devices.