标题： 魔角取向分子聚集体中激子输运的鲁棒表面增强 显示英文标题

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

摘要： 分子聚集体在魔角取向下的激子传输预计由于其可忽略的偶极-偶极相互作用而被强烈抑制。 然而，最近的报道表明，光-物质相互作用可以通过光子场介导的有效长程耦合显著增强激子传输。 为了阐明它们的相互作用，我们采用宏观量子电动力学框架来模拟一个染料分子阵列在靠近银表面的魔角配置中的激子传输。 我们的结果表明，激子扩散系数有显著增强，并且在染料分子-表面距离、分子间距离和分子跃迁频率变化时都具有鲁棒性。 此外，基于像偶极方法，我们推导出与数值模拟相符的解析表达式，揭示了这种增强来源于金属表面辐射散射引起的近场耦合项。 更重要的是，我们在金属表面附近的扩散系数尺度上观察到了与自由空间不同的非平凡差异。 我们的发现突显了通过设计耦合的激子-光子系统并工程化介电环境来控制激子传输的潜力。 显示英文摘要

摘要： 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.