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

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.

Mesoscale and Nanoscale Physics (cond-mat.mes-hall); Quantum Physics (quant-ph)

arXiv:2511.01723 [cond-mat.mes-hall]

(or arXiv:2511.01723v2 [cond-mat.mes-hall] for this version)

https://doi.org/10.48550/arXiv.2511.01723 Focus to learn more arXiv-issued DOI via DataCite

Phys. Rev. Lett. 137, 116901 (2026)

https://doi.org/10.1103/m138-4w64 Focus to learn more DOI(s) linking to related resources

arXivLabs is a framework that allows collaborators to develop and share new arXiv features directly on our website.

Both individuals and organizations that work with arXivLabs have embraced and accepted our values of openness, community, excellence, and user data privacy. arXiv is committed to these values and only works with partners that adhere to them.

Have an idea for a project that will add value for arXiv's community? Learn more about arXivLabs.