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| Autori principali: | , , , , |
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| Natura: | Preprint |
| Pubblicazione: |
2025
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| Soggetti: | |
| Accesso online: | https://arxiv.org/abs/2511.01723 |
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| _version_ | 1866914132888911872 |
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| author | Dherbécourt, Maxime Bellessa, Joël Symonds, Clémentine Weick, Guillaume Hagenmüller, David |
| author_facet | Dherbécourt, Maxime Bellessa, Joël Symonds, Clémentine Weick, Guillaume Hagenmüller, David |
| contents | 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 work 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2511_01723 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Spontaneous Raman Scattering under Vibrational Strong Coupling: The Critical Role of Polariton Spatial Mode Coherence Dherbécourt, Maxime Bellessa, Joël Symonds, Clémentine Weick, Guillaume Hagenmüller, David Mesoscale and Nanoscale Physics Quantum Physics 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 work 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. |
| title | Spontaneous Raman Scattering under Vibrational Strong Coupling: The Critical Role of Polariton Spatial Mode Coherence |
| topic | Mesoscale and Nanoscale Physics Quantum Physics |
| url | https://arxiv.org/abs/2511.01723 |