English

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

Chemical Physics 2026-07-16 v1 Statistical Mechanics

Abstract

Recent experiments by Sandeep \textit{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 coupled fields: a cavity-controlled collective vibrational polarization PP and a secondary structural field mm whose long-wavelength susceptibility is renormalized by the collective vibrational polarization intensity P2P^2, assumed to govern long-wavelength density/dielectric fluctuations. 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.

Keywords

Cite

@article{arxiv.2607.15497,
  title  = {A Mesoscopic Ginzburg--Landau Model for Vibrational Strong Coupling Enhanced Rayleigh Scattering in Molecular Liquids},
  author = {Wenxiang Ying and Abraham Nitzan},
  journal= {arXiv preprint arXiv:2607.15497},
  year   = {2026}
}

Comments

18 pages, 4 figures