A Mesoscopic Ginzburg--Landau Model for Vibrational Strong Coupling Enhanced Rayleigh Scattering in Molecular Liquids
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 P and a secondary structural field m whose long-wavelength susceptibility is renormalized by the collective vibrational polarization intensity P2, 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.
Versions
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BibTeX
@misc{ying2026mesoscopic,
title = {{A Mesoscopic Ginzburg--Landau Model for Vibrational Strong Coupling Enhanced Rayleigh Scattering in Molecular Liquids}},
author = {Wenxiang Ying and Abraham Nitzan},
howpublished = {arXiv},
year = {2026},
month = jul,
doi = {10.48550/arxiv.2607.15497},
eprint = {2607.15497},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2607.15497},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - A Mesoscopic Ginzburg--Landau Model for Vibrational Strong Coupling Enhanced Rayleigh Scattering in Molecular Liquids
AU - Wenxiang Ying
AU - Abraham Nitzan
PY - 2026
DA - 2026/07/16
PB - arXiv
DO - 10.48550/arxiv.2607.15497
UR - https://arxiv.org/abs/2607.15497
AB - 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 P and a secondary structural field m whose long-wavelength susceptibility is renormalized by the collective vibrational polarization intensity P^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.
ER -