Molecular optomechanics describes surface-enhanced Raman scattering using the formalism of cavity optomechanics as a parametric coupling of the molecule's vibrational modes to the plasmonic resonance. Most of the predicted applications require intense electric field hotspots but spectrally narrow resonances, out of reach of standard plasmonic resonances. The Fano lineshapes resulting from the hybridization of dielectric-plasmonic resonators with a broad-band plasmon and narrow-band cavity mode allow reaching strong Raman enhancement with high-Q resonances, paving the way for sideband resolved molecular optomechanics. We extend the molecular optomechanics formalism to describe hybrid dielectric-plasmonic resonators with multiple optical resonances and with both free-space and waveguide addressing. We demonstrate how the Raman enhancement depends on the complex response functions of the hybrid system, and we retrieve the expression of Raman enhancement as a product of pump enhancement and the local density of states. The model allows prediction of the Raman emission ratio into different output ports and enables demonstrating a fully integrated high-Q Raman resonator exploiting multiple cavity modes coupled to the same waveguide.

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ACS
The Netherlands Organisation for Scientific Research (NWO) , European Union Horizon 2020 , European Research Council (ERC)
doi.org/10.1021/acsphotonics.1c00808
ACS Photonics
Resonant Nanophotonics

Shlesinger, I, Cognée, K.G, Verhagen, E, & Koenderink, A.F. (2021). Integrated Molecular Optomechanics with Hybrid Dielectric-Metallic Resonators. ACS Photonics, 8(12), 3506–3516. doi:10.1021/acsphotonics.1c00808