Chasing Vibro-Polariton Fingerprints in Infrared and Raman Spectra Using Surface Lattice Resonances on Extended Metasurfaces

[Image: see text] We present an experimental investigation of vibrational strong coupling of C=O bonds in poly(methyl methacrylate) to surface lattice resonances (SLRs) on arrays of gold particles in infrared and Raman spectra. SLRs are generated from the enhanced radiative coupling of localized resonances in single particles by diffraction in the array. Compared to previous studies in Fabry–Perot cavities, particle arrays provide a fully open system that easily couples with external radiation while having large field confinement close to the array. We control the coupling by tuning the period of the array, as evidenced by the splitting of the C=O vibration resonance in the lower and upper vibro-polaritons of the IR extinction spectra. Despite clear evidence of vibrational strong coupling in IR transmission spectra, both Raman spectroscopy and micro-Raman mapping do not show any polariton signatures. Our results suggest that the search for vibrational strong coupling in Raman spectra may need alternative cavity designs or a different experimental approach.