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arXiv 2607.15497physics.chem-phcond-mat.stat-mech

分子液体中振动强耦合增强瑞利散射的介观金兹堡 - 朗道模型

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

Wenxiang Ying, Abraham Nitzan

AI总结:

研究分子液体中振动强耦合增强瑞利散射,构建介观金兹堡 - 朗道模型,含两个耦合场,校准参数后能捕捉相关现象并做出预测,为实验测试提供方向。

AI中文摘要:

桑迪普等人的近期实验表明分子液体中的振动强耦合(VSC)能产生超越单分子可观测的介观现象。受此启发,构建了一个具有两个耦合场的介观金兹堡 - 朗道模型,包括腔控集体振动极化\(P\)和二级结构场\(m\)。校准参数后,模型捕捉到了观测到的瑞利增强等现象,还预测了强瑞利增强区域的一些特性,可通过相关散射探针进行直接实验测试。

英文摘要:

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.

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