Journal
PHYSICAL REVIEW A
Volume 94, Issue 2, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevA.94.023843
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Funding
- EPSRC CM-CDT [EP/L015110/1]
- EPSRC program Hybrid Polaritonics [EP/M025330/1]
- Leverhulme Trust [IAF-2014-025]
- Engineering and Physical Sciences Research Council [EP/M025330/1, 1654073] Funding Source: researchfish
- EPSRC [EP/M025330/1] Funding Source: UKRI
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Strong coupling between cavity photons and molecular vibrations can lead to the formation of vibron-polaritons. In a recent experiment with PVAc molecules in a metal-metal microcavity [Shalabney et al., Angew. Chem., Int. Ed. 54, 7971 (2015)], such a coupling was observed to enhance the Raman scattering probability by several orders of magnitude. Inspired by this, we theoretically analyze the effect of strong photon-vibron coupling on the Raman scattering amplitude of organic molecules. This problem has recently been addressed by del Pino, Feist, and Garcia-Vidal [J. Phys. Chem. C 119, 29132 (2015)] using exact numerics for a small number of molecules. In this paper we derive compact analytic results for any number of molecules, also including the ultrastrong-coupling regime. Our calculations predict a division of the Raman signal into upper and lower polariton modes, with some enhancement to the lower polariton Raman amplitude due to the mode softening under strong coupling.
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