Nonadiabatic charge dynamics in novel solar cell materials

The review describes recent research into the nonequilibrium phenomena in nanoscale materials, with focus on charge separation and recombination, that form the basis for photovoltaic and photocatalytic devices. Nonadiabatic molecular dynamics combined with ab initio real‐time time‐dependent density functional theory enable us to model time‐resolved laser experiments at the atomistic level, emphasizing realistic aspects of the materials, such as defects, dopants, boundaries, chemical bonding, etc. A variety of systems have been considered, including bulk semiconductors sensitized by semiconducting/metallic nanoparticles and graphene, nanocrystal/molecule junctions, polymer interfaces with carbon nanotubes and nanoclusters, van der Waals heterojunctions, black phosphorus, and hybrid organic–inorganic perovskites. The detailed atomistic knowledge obtained from the explicit time‐domain modeling generates comprehensive understanding of electron‐vibrational dynamics in complex multi‐component systems, provides critical insights into quantum mechanical transport of energy and charge, and leads to valuable guidelines for improvement of solar‐to‐electric power conversion in photovoltaic and photocatalytic applications and for efficient performance of transport devices. WIREs Comput Mol Sci 2017, 7:e1305. doi: 10.1002/wcms.1305 This article is categorized under: Structure and Mechanism > Computational Materials Science