Broadband coherent Raman scattering spectroscopy at 50,000,000 spectra/s

Raman scattering spectroscopy is widely used as an analytical technique in various fields, but its measurement process tends to be slow due to the low scattering cross-section. In the last decade, various broadband coherent Raman scattering spectroscopy techniques have been developed to address this limitation, achieving a measurement rate of about 100 kSpectra/s. Here, we present a significantly increased measurement rate of 50 MSpectra/s, which is 500 times higher than the previous state-of-the-art, by developing time-stretch coherent Raman scattering spectroscopy. Our newly-developed system, based on a mode-locked Yb fiber laser, enables highly-efficient broadband excitation of molecular vibrations via impulsive stimulated Raman scattering with an ultrashort femtosecond pulse and sensitive time-stretch detection with a picosecond probe pulse at a high repetition rate of the laser. As a proof-of-concept demonstration, we measure broadband coherent Stokes Raman scattering spectra of organic compounds covering the molecular fingerprint region from 200 to 1,200 cm-1. This high-speed broadband vibrational spectroscopy technique holds promise for unprecedented measurements of sub-microsecond dynamics of irreversible phenomena and extremely high-throughput measurements.