Physical limits on Raman scattering: the critical role of pump and signal co-design

We present a method for deriving limits on Raman scattering in structured media and exploit it to constrain the maximum Raman signal resulting from a planewave incident on either a single Raman molecule in the vicinity of a structured medium or a designable Raman medium. Results pertaining to metallic and dielectric structures illustrate the importance of accounting for the nonlinear interplay between pump and signal fields, showing that treating the pump-focusing and signal-extraction processes separately, as in prior work, leads to unrealistic enhancements. The formulation could readily find applications in further enhancing surface-enhanced Raman scattering (SERS) spectroscopy and Raman-assisted lasing.