Quantum Dynamics of Photogenerated Charge Carriers in Hybrid Perovskites: Dopants, Grain Boundaries, Electric Order, and Other Realistic Aspects

Dissipation of photon energy to heat and recombination of photogenerated charge carriers are among the main factors limiting the efficiency of solar-light-harvesting devices. The dynamics of excited electrons and holes depends critically on the microscopic structure of a material, including dopants, defects, grain boundaries, crystallinity, and electric order. This Perspective summarizes recent findings and suggests directions for improvement of hybrid organic–inorganic perovskite materials, established by means of nonadiabatic dynamics (NAMD) simulations. Combined with real-time time-dependent density functional theory, NAMD provides an ab initio description of the photoinitiated processes that occur far from thermodynamic equilibrium. It includes realistic aspects of the material’s structure and gives unique atomistic insights into the photoactive material properties.