Addressing intramolecular vibrational redistribution in a single molecule through pump and probe surface-enhanced vibrational spectroscopy
This paper establishes a quantum mechanical framework based on molecular optomechanics to demonstrate that pump-and-probe surface-enhanced vibrational spectroscopy can detect intramolecular vibrational redistribution (IVR) signatures in single molecules through anti-Stokes SERS spectra, regardless of whether the vibrational pumping is driven by infrared lasers or Stokes scattering.