Multiscale Simulations and Property Predictions for Organic Luminescent Aggregates

ABSTRACT Precise regulation of aggregation‐state luminescence is a crucial and challenging task in the field of organic luminescence. The luminescence properties of organic molecular aggregates are intricately governed by both molecular conformations and intermolecular packing structures. The inherent conformational flexibility and the cooperative interplay of diverse intermolecular interactions in organic molecular aggregates give rise to numerous kinetically stable states besides the thermodynamically stable state, as well as multi‐level couplings associated with excited states, which make the prediction of luminescent properties extraordinarily complicated and challenging. In this review, we first introduce a general theoretical protocol that combines multiscale modeling, kinetic network model, and excited‐state decay rate theory. Then, the mechanism of luminescence and its regulation are presented for various organic molecular aggregates ranging from homogenous crystals, cocrystals, heterogenous amorphous aggregates, to kinetically controlled assemblies. Importantly, the mapping relationship is established between the formation processes of organic molecular aggregates and the corresponding dynamic luminescent properties, which provide valuable insights for a deeper understanding of aggregation‐state luminescent properties and facilitate the precise regulation of organic luminescent materials.