Robust Surface-Induced Enhancement of Exciton Transport in Magic-Angle-Oriented Molecular Aggregates

• URL: http://arxiv.org/abs/2507.13755v1
• Date: Fri, 18 Jul 2025 08:59:48 GMT
• Title: Robust Surface-Induced Enhancement of Exciton Transport in Magic-Angle-Oriented Molecular Aggregates
• Authors: Siwei Wang, Liang-Yan Hsu, Hsing-Ta Chen,
• Abstract summary: Recent reports show that light-matter interactions can significantly enhance exciton transport.<n>We simulate exciton transport within a chromophore array arranged in a magic-angle configuration in proximity to a silver surface.
• Score: 23.22864925146285
• License: http://creativecommons.org/licenses/by/4.0/
• 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 diffusion coefficient 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 non-trivial differences in the diffusion coefficient's scaling 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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