From Molecular Packing Structures to Electronic Processes: Theoretical Simulations for Organic Solar Cells

Abstract Molecular packing structures in the active layers have a crucial impact on the electronic processes for organic solar cells. To date, however, it is still difficult to probe molecular self‐assembling and packing structures at the atomic level by experimental techniques, which is hindering reliable understanding of the structure–property relationship. Accordingly, theoretical simulations provide a useful tool and are becoming more and more important. Here, recent advances in theoretical simulations for organic solar cells are reviewed. First, a brief introduction of theoretical methodologies, including the strategies of molecular dynamics simulations of active‐layer processing procedures and quantum‐chemical methods for calculating electron transfer processes, is given. Then, the influences of molecular packing structures on charge generation, charge recombination, and charge transport are analyzed and discussed from a theoretical perspective. Finally, prospects and challenges are pointed out for theoretical prediction of the electrical characteristics and photoelectric conversion efficiencies of organic solar cells from molecular structures.