Disorder-Induced Spectral Splitting versus Rabi Splitting under Strong Light-Matter Coupling
arXiv:2411.03479 · doi:10.1021/acs.jpclett.5c01302
Abstract
The notion of strong light-matter coupling is typically associated with the observation of Rabi splitting, corresponding to the formation of the hybrid light-matter states known as polaritons. However, this relationship is derived based on the assumption that disorder can be ignored or acts as a perturbative effect. Contrary to conventional treatment of disorder effects, we investigate the impact of strong disorder on the absorption spectrum by developing a non-perturbative effective model combined with classical electrodynamics simulation. Intriguingly, we find that strong disorder leads to an enhanced spectral splitting that closely resembles Rabi splitting, yet originates from a fundamentally different mechanism as induced by the dark modes. Specifically, we examine a disordered molecular ensemble in proximity to a plasmonic nanodisk and demonstrate disorder-induced spectral splitting in the absorption spectrum. This conclusion raises a controversial issue, suggesting that both polaritons (dominate in the strong coupling regime) and dark modes (dominate in the strong disorder regime) can lead to spectral splitting, and one cannot distinguish them solely based on the steady-state absorption spectrum.
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