In this chapter, the focus lies with the use of stimulated Raman scattering (SRS) to image brain tissue, allowing for accurate and spatially precise tumor detection. Raman spectroscopy, a method which relies on the vibrational states of molecules within a sample to determine its chemical composition based on how molecular bonds interact with incident light, has shown promise for this application. Raman spectroscopy provides a means of differentiating tumor from normal brain based on chemical content. Broadband coherent anti-Stokes Raman Scattering microscopy is the most similar technology to SRS being investigated for neurosurgical application. Like SRS, it is a coherent Raman imaging modality, and is thus able to generate images of tissue histoarchitecture based on chemical composition. The clinical adoption of SRS microscopy had been hindered by the need for a robust, tunable laser with an ultrafast, dual-wavelength source. Until recently, a synchronously pumped picosecond optical parametric oscillator has been the gold standard source for SRS microscopy.