Delocalization versus Coherence under Vibrational and Environmental Disorder in Photoexcited Supramolecular Aggregates.

ABSTRACT: Exciton and charge dynamics in photoexcited molecular materials depend critically on how delocalization competes with structural, vibrational, and environmental disorder. Yet, the origin and extent of coherent versus incoherent distribution of excitons and charges in such "noisy" supramolecular systems remain poorly understood. Here, we integrate all-atom classical dynamics with fully quantum vibronic dynamics to dissect these competing effects in aqueous self-assembled perylenediimide stacks. Our simulations quantitatively reproduce experimental absorption spectra and reveal that strong excitonic coupling and hybridization with charge-transfer states dictate the optical response. Following photoexcitation, the electronic populations rapidly spread across multiple molecules within tens of

SUBMITTER: Giannini S 

PROVIDER: S-EPMC12856889 | biostudies-literature | 2026 Jan

REPOSITORIES: biostudies-literature