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Updated: Jan 16, 2026

Excitonic Hamiltonians for Calculating Optical Absorption Spectra and Optoelectronic Properties of Molecular Aggregates and Solids
Published on: May 27, 2020
Robust Surface-Induced Enhancement of Exciton Transport in Magic-Angle-Oriented Molecular Aggregates
Siwei Wang1, Liang-Yan Hsu2,3,4, Hsing-Ta Chen1
1Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556, United States.
Abstract:
Exciton transport in molecular aggregates with magic-angle orientation is expected to be strongly suppressed due to their negligible dipole-dipole interactions. However, recent reports show that light-matter interactions can significantly enhance exciton transport, attributed to the effective long-range coupling mediated by the photonic fields. To elucidate their interplay, we employ the macroscopic quantum electrodynamics framework to simulate exciton transport within a chromophore array arranged in a magic-angle configuration in proximity to a silver surface. Our results show a significant enhancement of the exciton mean square velocity that is robust across variations in chromophore-surface separation, intermolecular distance, and molecular transition frequency. Furthermore, based on the image-dipole method, we derive analytical expressions that agree well with numerical simulations, revealing the enhancement's origin in the near-field coupling term as induced by the radiative scattering at the metallic surface. More importantly, we observe nontrivial differences in the power-law scaling of the mean square velocity near metallic surfaces compared to free space. Our findings highlight the potential to control exciton transport by designing coupled exciton-photon systems and engineering the dielectric environments.
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