Broadband Coherent Raman Scattering Spectroscopy at 50,000,000 Spectra per Second

Abstract

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 500 kSpectra/s. Here, we present a substantially increased measurement rate of 50 MSpectra/s, which is 100 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.