Complementary Vibrational Spectroscopy

Abstract: Vibrational spectroscopy, comprised of infrared absorption and Raman scattering spectroscopy, is widely used for label-free optical sensing and imaging in various scientific and industrial fields. The group theory states that the two molecular spectroscopy methods are sensitive to vibrations categorized in different point groups and provide complementary vibrational spectra. Therefore, complete vibrational information cannot be acquired by a single spectroscopic device, which has impeded the full potential of vibrational spectroscopy. Here, we demonstrate simultaneous infrared absorption and Raman scattering spectroscopy that allows us to measure the complete broadband vibrational spectra in the molecular fingerprint region with a single instrument based on an ultrashort pulsed laser. The system is based on dual-modal Fourier-transform spectroscopy enabled by efficient use of nonlinear optical effects. Our proof-of-concept experiment demonstrates rapid, broadband and high spectral resolution measurements of complementary spectra of organic liquids for precise and accurate molecular analysis.