Disorder-Induced Spectral Splitting versus Rabi Splitting under Strong Light-Matter Coupling

TL;DR

This paper demonstrates that strong disorder in a molecular ensemble can cause spectral splitting similar to Rabi splitting, but through a different mechanism involving dark modes, challenging the conventional interpretation of spectral features in strong light-matter coupling.

Contribution

It introduces a non-perturbative model showing disorder-induced spectral splitting, distinguishing it from Rabi splitting caused by polaritons, and highlights the role of dark modes.

Findings

Disorder can induce spectral splitting resembling Rabi splitting.

Dark modes can dominate spectral features in strong disorder regimes.

Spectral splitting alone cannot distinguish between polaritons and dark mode effects.

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.