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

Maxime Dherbécourt1, Joël Bellessa2,*, Clémentine Symonds2, Guillaume Weick1,†, and David Hagenmüller1,‡

  • *Contact author: joel.bellessa@univ-lyon1.fr
  • †Contact author: guillaume.weick@ipcms.unistra.fr
  • ‡Contact author: david.hagenmuller@ipcms.unistra.fr
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Phys. Rev. Lett. 137, 116901 – Published 8 September, 2026

DOI: https://doi.org/10.1103/m138-4w64

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.

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Phys. Rev. Lett. 137, 116901– Published 8 September, 2026
  • Received 10 November 2025
  • Accepted 22 July 2026
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