Ultra-high-speed coherent anti-Stokes Raman spectroscopy with a hybrid dual-comb source

Abstract: Coherent anti-Stokes Raman scattering (CARS) spectroscopy with time-delayed ultrashort pulses and a single-pixel photodetector has shown great potential for spectroscopic imaging and transient studies in chemistry and biological research. However, those systems rely on mechanical delay lines or two asynchronous optical combs with inflexible repetition frequencies, technically limiting their acquisition speeds. Here, we demonstrate a hybrid dual-comb CARS system involving a broadband fiber laser and a highly-flexible, frequency-modulated electro-optic comb. We achieve multiplex CARS spectra (2800-3200 cm-1), with a moderate resolution (22 cm-1), at a maximum refresh rate of 1 MHz, limited by the radio-frequency synthesizer we use. Fast spectroscopic CARS imaging is demonstrated for liquid mixtures. Our system enables spectral measurements in the high-wavenumber C-H stretching region at a record speed that is an order of magnitude higher than state-of-the-art systems, which may open up new opportunities for fast chemical sensing and imaging.