Coherent versus incoherent Raman scattering: molecular coherence excitation and measurement.
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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 10(5)-fold increase in the efficiency of the Raman scattering process due to the broadband pump-Stokes preparation. The coherence magnitude (approximately 0.5x10(-3)) is inferred experimentally, without a priori knowledge about the molecular structure.
author list (cited authors)
Pestov, D., Ariunbold, G. O., Wang, X. i., Murawski, R. K., Sautenkov, V. A., Sokolov, A. V., & Scully, M. O.