Generating Coherent Raman Scattering Using a Molecular Optomechanical Cavity

Coherent Raman scattering, e.g., coherent anti-Stokes Raman scattering (CARS) and stimulated Raman scattering (SRS), has emerged as a powerful tool for label-free molecular imaging in biological and biomedical systems. Here we develop an optomechanical approach for coherent Raman spectroscopy with a focus on the CARS and SRS. The results show that the Raman cross section can be significantly enhanced by increasing the pump strength. It turns out that the CARS signal is robust to the external temperature, yielding an order of magnitude amplification due to √N collectivity. We further find that the power spectrum of the emission is dominated by the SRS process. The SRS signal presents an anti-Stokes component appreciably stronger than the Stokes one. Our work suggests a new scheme for generating coherent Raman signals with enhanced stability and signal-to-noise ratio, which would be beneficial for molecular spectroscopy. © 2025 The Authors. Published by American Chemical Society.