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Spectral analysis of high-order harmonics generated by ultrashort mid-infrared pulses in molecular nitrogen reveals well-resolved signatures of inverse Raman scattering, showing up near the frequencies of prominent vibrational transitions of nitrogen molecules. When tuned on a resonance with the vʹ = 0 → vʺ = 0 pathway within the B3Πg → C3Πu second positive system of molecular nitrogen, the eleventh harmonic of a 3.9-μm sub-80-fs driver is shown to acquire a distinctive antisymmetric spectral profile with red-shifted bright and blue-shifted dark features as indicators of stimulated Raman gain and loss. This high-harmonic setting extends the inverse Raman effect to a vast class of strong-field light–matter interaction scenarios.
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Alexei M. Zheltikov, Mitrofanov Alexander, Dmitri Sidorov-Biryukov, Alexander Voronin, Rozhko Mikhail, Andrey Fedotov, "High-harmonic inverse Raman scattering," Proc. SPIE 11770, Nonlinear Optics and Applications XII, 117700I (19 April 2021); https://doi.org/10.1117/12.2592673