Photoinduced Dynamics of Charge Carriers in Metal Halide Perovskites from an Atomistic Perspective

Perovskite solar cells have attracted intense attention over the past decade because of their low cost, abundant raw materials, and rapidly growing power conversion efficiency (PCE). However, nonradiative charge carrier losses still constitute a major factor limiting the PCE to well below the Shockley–Queisser limit. This Perspective summarizes recent atomistic quantum dynamics studies on the photoinduced excited-state processes in metal halide perovskites (MHPs), including both hybrid organic–inorganic and all-inorganic MHPs and three- and two-dimensional MHPs. The simulations, performed using a combination of time-domain ab initio density functional theory and nonadiabatic molecular dynamics, allow emphasis on various intrinsic and extrinsic features, such as components, structure, dimensionality and interface engineering, control and exposure to various environmental factors, defects, surfaces, and their passivation. The detailed atomistic simulations advance our understanding of electron–vibrational dynamics in MHPs and provide valuable guidelines for enhancing the performance of perovskite solar cells.