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Plasmon resonances at the surface of plasmonic antennas allow for extremelystrong enhancement of Raman scattering. Intrinsic to plasmonics, however, isthat extreme field confinement lacks precise spectral control, which would holdgreat promise in shaping the optomechanical interaction between light andmolecular vibrations at will. We demonstrate an experimental platform composedof a plasmonic nanocube-on-mirror antenna coupled to an open, tunableFabry-Perot microcavity for selective addressing of individual vibrationallines of molecules with strong Raman scattering enhancement. Multiple narrowand intense optical resonances arising from the hybridization of the cavitymodes and the plasmonic broad resonance are used to simultaneously enhance thelaser pump and the local density of optical states (LDOS) and are characterizedusing rigorous modal analysis. The versatile bottom-up fabrication approachpermits quantitative comparison with the bare nanocube-on-mirror system, boththeoretically and experimentally. This shows that the hybrid system allows forsimilar SERS enhancement ratios with narrow optical modes, paving the way fordynamical back action effects in molecular optomechanics.

Hybrid cavity-antenna architecture for strong and tunable sideband-selective molecular Raman scattering enhancement