Mode-Specific Coupling of Nanoparticle-on-Mirror Cavities with Cylindrical Vector Beams

Nano Lett. 2023 Jun 14;23(11):4885-4892. doi: 10.1021/acs.nanolett.3c00561. Epub 2023 May 19.

Abstract

Nanocavities formed by ultrathin metallic gaps permit the reproducible engineering and enhancement of light-matter interaction, with mode volumes reaching the smallest values allowed by quantum mechanics. While the enhanced vacuum field in metallic nanogaps has been firmly evidenced, fewer experimental reports have examined the far-field to near-field input coupling under strongly focused laser beam. Here, we experimentally demonstrate selective excitation of nanocavity modes controlled by the polarization and frequency of the laser beam. We reveal mode selectivity by recording confocal maps of Raman scattering excited by cylindrical vector beams, which are compared to the known excitation near-field patterns. Our measurements reveal the transverse vs longitudinal polarization of the excited antenna mode and how the input coupling rate depends on laser wavelength. The method introduced here is easily applicable to other experimental scenarios, and our results help connect far-field with near-field parameters in quantitative models of nanocavity-enhanced phenomena.

Keywords: Cylindrical vector beams; Near-field; Plasmonic antennas; Plasmonic cavities; Surface-enhanced Raman scattering.