Super-broadband stimulated Raman scattering spectroscopy and imaging

Raman spectroscopy is a valuable tool widely used in biology and medicine. While still serving as the mainstream approach for high-fidelity Raman spectral analysis and imaging, spontaneous Raman scattering suffers from low acquisition speed and fluorescence interference. Here we report super-broadband stimulated Raman scattering (SuperB-SRS), a technique able to provide identical spectra to state-of-the-art spontaneous Raman over thousands of wavenumber ranges while being orders of magnitude faster and naturally supporting simultaneous multiplexed fluorescence detection. SuperB-SRS encodes the ideal Raman free induction decays into the stimulated Raman loss through few-cycle laser-induced quantum interference, permitting universal Raman analysis and imaging that unites high spectral fidelity, natural-linewidth-limited spectral resolution, broad bandwidth and state-of-the-art sensitivity. We demonstrate more than a 100-fold increase in speed for imaging of biological tissue samples compared with spontaneous Raman. As a medical application, we detect in clinical serum samples 11 biomarkers widely used to assess liver and kidney functions, cardiovascular diseases and other conditions. SuperB-SRS thus enables generating high-quality, large-scale datasets for data-driven health science, promising wide applications in multiple fields of science.