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Label-free Raman-based imaging techniques create the possibility of bringing chemical and histologic data into the operation room. Relying on the intrinsic biochemical properties of tissues to generate image contrast and optical tissue sectioning, Raman-based imaging methods can be used to detect microscopic tumor infiltration and diagnose brain tumor subtypes. Here, we review the application of three Raman-based imaging methods to neurosurgical oncology Raman spectroscopy, coherent anti-Stokes Raman scattering (CARS) microscopy, and stim