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

• URL: http://arxiv.org/abs/2511.01723v1
• Date: Mon, 03 Nov 2025 16:33:38 GMT
• Title: 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,
• Abstract summary: In a homogeneously filled cavity, spatial overlap between polaritons and cavity resonances enforces selection rules.<n>For a quasi-two-dimensional (2d) molecular layer, these rules are lifted, yielding Raman peaks at the polariton energies.<n>Our work clarifies that the Raman response under vibrational strong coupling is determined by cavity-vibration spatial mode overlap.
• Score: 0.0
• License: http://creativecommons.org/licenses/by/4.0/
• 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 work 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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