We present a comparative analysis of spontaneous and coherent Raman scattering on pyridine. The instantaneous excitation of the molecular coherence is done by a pair of ultrashort preparation pulses. Then, a long narrowband probe pulse is scattered off the molecular vibrations. The described hybrid technique allows for the single-shot acquisition of a background-free coherent Raman spectrum within the excitation band and its straightforward comparison with the spontaneous Raman measurements, performed in the same setup. We report a -fold increase in the efficiency of the Raman scattering process due to the broadband pump–Stokes preparation. The coherence magnitude is inferred experimentally, without a priori knowledge about the molecular structure.
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