Disorder-Induced Localization of Molecular Polaritons Despite Spectroscopic Strong Coupling

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Original abstract

Molecular polaritons are hybrid light--matter quasiparticles whose collective character is often associated with molecular excitations extending over many emitters. However, molecular ensembles are intrinsically disordered and dissipative, and spectrally visible polariton peaks do not necessarily imply delocalized molecular character. Here, we theoretically examine how static energetic disorder and finite cavity and molecular linewidths affect the delocalization of electronic polaritons in cavity--coupled molecular ensembles. Using a disordered Tavis--Cummings model, we show that energetic disorder mixes polariton states with the dark-state manifold, causing a rapid loss of collective molecular character even when polaritonic spectral features remain visible. We quantify this crossover using the molecular participation ratio, a density--matrix--based coherence measure, and an energy--resolved autocorrelation function. In the lossless electronic model, preserving an extended polaritonic molecular component requires the collective Rabi splitting to exceed the disorder width by more than a factor of five, providing a stricter condition than conventional spectroscopic strong coupling. Extending the analysis to a non--Hermitian Hamiltonian shows that cavity--molecule linewidth imbalance further reduces disorder tolerance. The resulting delocalization boundary indicates that preserving an extended molecular polariton component requires a collective Rabi splitting larger than roughly eight times the disorder width plus approximately twice the cavity--molecule linewidth mismatch. These results provide a quantitative criterion for polariton delocalization under disorder and loss and show that disorder, dissipation, and collective coupling must be considered together when assessing whether molecular polaritons remain collectively extended in realistic optical cavities.

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• Official / arXiv page
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