Spontaneous Raman Scattering under Vibrational Strong Coupling: The Critical Role of Polariton Spatial Mode Coherence.

Authors

Maxime Dherbécourt, Joël Bellessa, Clémentine Symonds, Guillaume Weick, David Hagenmüller

Published in

Physical review letters. Volume 137. Issue 11. Pages 116901. Sep 11, 2026.

Abstract

Resonant coupling of a vibration to a cavity mode has been reported to dramatically modify spontaneous Raman scattering, but subsequent studies have produced conflicting results. In this Letter, we develop a microscopic quantum framework that captures the spatial structure of polaritonic modes. In a homogeneously filled cavity, spatial overlap between polaritons and cavity resonances enforces selection rules that suppress the initially reported polaritonic Raman peaks, consistent with most experiments. In contrast, for a quasi-two-dimensional (2D) molecular layer, these rules are lifted, yielding Raman peaks at the polariton energies. Our Letter clarifies that the Raman response under vibrational strong coupling is determined by cavity-vibration spatial mode overlap and offers a framework for Raman studies of strongly coupled quasi-2D systems.

PMID:
42789870
Bibliographic data and abstract were imported from PubMed on 26 Sep 2026.

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