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Plasmonic dimer cavities can induce extreme electric-field hot spots thatallow one to access ultrastrong coupling regimes using Raman-type spectroscopyon single vibrating molecules. Using a generalized master equation, we studyresonant Raman scattering in the strong coupling regime of cavity-QED, whenalso in the vibrational ultrastrong coupling regime, leading to "phonon-dressedpolaritons". The master equation rigorously includes spectral baths for thecavity and vibrational degrees of freedom, as well as a pure dephasing bath forthe resonant two-level system, which play a significant role. Employingrealistic parameters for gold dimer cavity modes, we investigate the emissionspectra in several characteristic strong-coupling regimes, leading to extremelyrich spectral resonances due to an interplay of phonon-modified polaritonstates and bath-induced resonances. We also show explicitly the failure of thestandard master equation in these quantum nonlinear regimes.

physical review. b./physical review. b

Resonant Raman scattering of single molecules under strong cavity  coupling and ultrastrong optomechanical coupling in plasmonic resonators:  phonon-dressed polaritons