Optomechanical Pumping of Collective Molecular Vibrations in Plasmonic Nanocavities.

ABSTRACT: In surface-enhanced Raman scattering (SERS), vibrations of molecules couple with optical modes of a plasmonic nanocavity via a molecular optomechanical interaction. This molecule-plasmon coupling gives rise to optomechanical effects such as vibrational pumping-the excitation of molecular vibrations due to Stokes scattering. Here, we investigate the influence of vibrational pumping and collective effects on biphenyl-4-thiol (BPT) molecules in nanoparticle-on-mirror nanocavities, both experimentally by pulsed SERS spectroscopy and theoretically with optomechanical modeling. From the anti-Stokes to Stokes ratio of hundreds of individual nanostructures, we provide clear experimental evidence of vibrational pumping in high-wavenumber vibrational modes at room temperature and investigate the eme

SUBMITTER: Jakob LA 

PROVIDER: S-EPMC11948455 | biostudies-literature | 2025 Mar

REPOSITORIES: biostudies-literature