Abstract
<jats:p>Shifted excitation Raman difference spectroscopy (SERDS) is a method for eliminating fluorescence in Stokes Raman spectra and serves as an alternative to computational pre-processing methods. However, the choice of the magnitude of the excitation laser frequency shift induces a systematic variation in the results. In this paper, we present a mathematical model that precisely describes how measured peak positions and heights depend on the choice of the frequency shift. The derived model can be used to assess systematic errors and signal-to-noise ratios in SERDS experiments, thereby assisting in selecting the optimal excitation frequency shift for a given application. We validate our findings with simulations and measurements of polystyrene.</jats:p>