Robust Surface-Induced Enhancement of Exciton Transport in Magic-Angle-Oriented Molecular Aggregates
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arXiv
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| Format: | Preprint |
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2025
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| author | Wang, Siwei Hsu, Liang-Yan Chen, Hsing-Ta |
| author_facet | Wang, Siwei Hsu, Liang-Yan Chen, Hsing-Ta |
| contents | 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2507_13755 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Robust Surface-Induced Enhancement of Exciton Transport in Magic-Angle-Oriented Molecular Aggregates Wang, Siwei Hsu, Liang-Yan Chen, Hsing-Ta Chemical Physics Quantum Physics 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. |
| title | Robust Surface-Induced Enhancement of Exciton Transport in Magic-Angle-Oriented Molecular Aggregates |
| topic | Chemical Physics Quantum Physics |
| url | https://arxiv.org/abs/2507.13755 |