A Mesoscopic Ginzburg–Landau Model for Vibrational Strong Coupling Enhanced Rayleigh Scattering in Molecular Liquids

Abstract

Recent experiments by Sandeep et al. [Angew. Chem. Int. Ed.65, e16917 (2026). ] suggest that vibrational strong coupling (VSC) in molecular liquids can generate mesoscopic phenomena beyond single-molecule observables, including resonantly enhanced Rayleigh scattering, abrupt concentration thresholds, and thermal collapse. Motivated by these observations, we construct a mesoscopic Ginzburg–Landau model with two biquadratically coupled coarse-grained fields: a cavity-controlled collective vibrational field, ϕP, and a secondary structural field, ϕm, assumed to govern long-wavelength density/dielectric fluctuations. At the mean-field level, the long-wavelength susceptibility of ϕm is renormalized by the coupling of ϕP. With calibrated parameters, the model captures the observed Rayleigh enhancement, collective scaling relations, and threshold-like behavior, while explaining why polaritonic/IR signatures may persist when Rayleigh scattering disappears. The model further predicts enhanced long-wavelength density/dielectric correlations, enlarged mesoscopic correlation lengths, and slowed structural dynamics in the regime with strong Rayleigh enhancement, providing direct experimental tests through small-angle X-ray/neutron scattering and dynamic light-scattering probes.