Static disorder-induced renormalization of polariton group velocity

Molecular exciton-polaritons exhibit long-range, ultrafast propagation, yet recent experiments have reported far slower propagation than expected. In this work, we implement a nonperturbative approach to quantify how static energetic disorder renormalizes polariton group velocity in strongly coupled microcavities. The method requires no exact diagonalization or master equation propagation and depends only on measurable parameters: the mean exciton energy and its probability distribution, the microcavity dispersion, and the Rabi splitting. Using parameters corresponding to recently probed organic microcavities, we show that exciton inhomogeneous broadening slows both lower and upper polaritons, particularly when the mean exciton energy fluctuation approaches the collective light-matter coupling strength. A detailed discussion and interpretation of these results is provided using perturbation theory in the limit of weak resonance scattering. The magnitude of the effects examined in this work supports the conclusion that most of the reported polaritonic slowdown arises from dynamical (phonon-assisted) disorder, with static energetic disorder contributing only secondarily.

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Publication Details

Journal
The Journal of Chemical Physics
Published
2025-09-25
DOI
https://doi.org/10.1063/5.0288551
Citations
1
Primary Topic
Strong Light-Matter Interactions
Type
article
Field-Weighted Citation Impact
1.25
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article

Static disorder-induced renormalization of polariton group velocity

Raphael F. Ribeiro, Gustavo J. R. Aroeira
1 citations
The Journal of Chemical Physics
Strong Light-Matter Interactions
1.25
article

Static disorder-induced renormalization of polariton group velocity

Raphael F. Ribeiro, Gustavo J. R. Aroeira
article en
1 citations

Abstract

Molecular exciton-polaritons exhibit long-range, ultrafast propagation, yet recent experiments have reported far slower propagation than expected. In this work, we implement a nonperturbative approach to quantify how static energetic disorder renormalizes polariton group velocity in strongly coupled microcavities. The method requires no exact diagonalization or master equation propagation and depends only on measurable parameters: the mean exciton energy and its probability distribution, the microcavity dispersion, and the Rabi splitting. Using parameters corresponding to recently probed organic microcavities, we show that exciton inhomogeneous broadening slows both lower and upper polaritons, particularly when the mean exciton energy fluctuation approaches the collective light-matter coupling strength. A detailed discussion and interpretation of these results is provided using perturbation theory in the limit of weak resonance scattering. The magnitude of the effects examined in this work supports the conclusion that most of the reported polaritonic slowdown arises from dynamical (phonon-assisted) disorder, with static energetic disorder contributing only secondarily.

The Journal of Chemical PhysicsVol. 163(12)
Emory University (US), Atlanta University Center (US)
Openalex Percentile: Top 17%
Strong Light-Matter Interactions
1.25
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