By using time-dependent density functional theory, we investigate in a fully quantum mechanical framework the interactions, in an ultra-near-field regime, between a localized surface plasmon excitable in a silver tetrahedral cluster and a molecular exciton with excitation energy in the same range. We show that, for metal–molecule distances below 5 Å, the optical response of the system results characterized by the appearance of a double peak structure. We analyze the transition densities for the resonant energies and propose a plasmon–exciton electromagnetic interaction model to explain the emerging of a lower energy resonance in the spectra of such kind of hybrid systems of interest for molecular plasmonics.

中文翻译：

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混合等离子体系统的原子研究

通过使用时间相关的密度泛函理论，我们在一个完全量子力学的框架中研究了在超近场范围内，在银四面体簇中可激发的局域表面等离子体与具有相同激发能量的分子激子之间的相互作用。范围。我们表明，对于低于 5 Å 的金属-分子距离，系统结果的光学响应表现为双峰结构的出现。我们分析了共振能量的跃迁密度，并提出了一个等离子体-激子电磁相互作用模型来解释在这种对分子等离子体感兴趣的混合系统的光谱中出现低能量共振。