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 two molecular spectroscopy methods are sensitive to different types of vibrations and provide complementary vibrational spectra, but obtaining complete vibrational information with a single spectroscopic device is challenging due to the large wavelength discrepancy between the two methods. 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.

Nature Communications 10, 4411 (2019),  UTokyoFOCUS

Flow cytometry is an indispensable tool in biology for counting and analyzing single cells in large heterogeneous populations. However, it predominantly relies on fluorescent labeling to differentiate cells and, hence, comes with several fundamental drawbacks. Here, we present a high-throughput Raman flow cytometer on a microfluidic chip that chemically probes single live cells in a label-free manner. It is based on a rapid-scan Fourier-transform coherent anti-Stokes Raman scattering spectrometer as an optical interrogator, enabling us to obtain the broadband molecular vibrational spectrum of every single cell in the fingerprint region (400 to 1600 cm−1) with a record-high throughput of ~2000 events/s. As a practical application of the method not feasible with conventional flow cytometry, we demonstrate high-throughput label-free single-cell analysis of the astaxanthin productivity and photosynthetic dynamics of Haematococcus lacustris.

Science Advances 5, aau0241 (2019)

Fourier-transform spectroscopy (FTS) has been widely used as a standard analytical technique over the past half-century. FTS is an autocorrelation-based technique that is compatible with both temporally coherent and incoherent light sources, and functions as an active or passive spectrometer. However, it has been mostly used for static measurements due to the low scan rate imposed by technological restrictions. This has impeded its application to continuous rapid measurements, which would be of significant interest for a variety of fields, especially when monitoring of non-repeating or transient complex dynamics is desirable. Here, we demonstrate highly efficient FTS operating at a high spectral acquisition rate with a simple delay line based on a dynamic phase-control technique. The independent adjustability of phase and group delays allows us to achieve the Nyquist-limited spectral acquisition rate over 10,000 spectra per second, while maintaining a large spectral bandwidth and high resolution. We also demonstrate passive spectroscopy with an incoherent light source.

Nature Communications 9, 4448 (2018)

We demonstrate ultra-broadband Fourier-transform coherent anti-Stokes Raman scattering (FT-CARS) spectroscopy spanning over 3,000 cm−1 with a rapid-scan Michelson interferometer at a scan rate of 24,000 spectra/s. Using sub-10-fs optical pulses from a mode-locked laser, we measure broad CARS spectrum covering both the fingerprint region (500-1,800 cm−1) and the C-H, N-H, O-H stretching region (2,700-3,600 cm−1). To the best of our knowledge, this is the first demonstration of coherent Raman scattering spectroscopy covering over 3,000 cm−1 at a scan rate of more than 10,000 spectra/s. Our system holds the potential for high-speed or high-throughput label-free chemical analysis, such as investigating non-repetitive chemical dynamics, taking large area images of materials or biological specimens, or counting and sorting a large number of heterogeneous cells.

Optics Express 26, 14307-14314 (2018)