Enriching molecular Raman spectroscopy with vibrational strong coupling
Abstract
Raman spectroscopy is widely used for molecular identification in biological samples, but spectral congestion often obscures key molecular fingerprints. Strategies to enrich vibrational spectra with additional controllable features are therefore desirable. We theoretically show that vibrational strong coupling (VSC) can reshape Raman spectra by reorganizing vibrational energies and intensities. Near-resonant coupling enables the resolution of quasi-degenerate vibrational modes and redistributes Raman activity among molecular vibrations, brightening otherwise Raman-inactive modes. Off-resonant coupling mediates effective interactions between vibrations, leading to tunable intensity reorganizations and spectral shifts via cavity-controlled vibrational mixing. Using a microscopic theory of Raman scattering, we show that observing Raman signals from collective VSC polaritons requires appropriate geometries for the scattering setup, the sample, and the cavity environment, helping to explain why polaritonic Raman signatures have remained challenging to observe experimentally.
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BibTeX
@misc{castagnola2026enriching,
title = {{Enriching molecular Raman spectroscopy with vibrational strong coupling}},
author = {Matteo Castagnola and Anne Todsen Hansen and Morten Hanefeld Dziegiel and Anders Kristensen and Søren Raza and Simone Latini},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.21542},
eprint = {2609.21542},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.21542},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Enriching molecular Raman spectroscopy with vibrational strong coupling
AU - Matteo Castagnola
AU - Anne Todsen Hansen
AU - Morten Hanefeld Dziegiel
AU - Anders Kristensen
AU - Søren Raza
AU - Simone Latini
PY - 2026
DA - 2026/09/18
PB - arXiv
DO - 10.48550/arxiv.2609.21542
UR - https://arxiv.org/abs/2609.21542
AB - Raman spectroscopy is widely used for molecular identification in biological samples, but spectral congestion often obscures key molecular fingerprints. Strategies to enrich vibrational spectra with additional controllable features are therefore desirable. We theoretically show that vibrational strong coupling (VSC) can reshape Raman spectra by reorganizing vibrational energies and intensities. Near-resonant coupling enables the resolution of quasi-degenerate vibrational modes and redistributes Raman activity among molecular vibrations, brightening otherwise Raman-inactive modes. Off-resonant coupling mediates effective interactions between vibrations, leading to tunable intensity reorganizations and spectral shifts via cavity-controlled vibrational mixing. Using a microscopic theory of Raman scattering, we show that observing Raman signals from collective VSC polaritons requires appropriate geometries for the scattering setup, the sample, and the cavity environment, helping to explain why polaritonic Raman signatures have remained challenging to observe experimentally.
ER -