Coherent versus incoherent Raman scattering: molecular coherence excitation and measurement |
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Authors: | Pestov Dmitry Ariunbold Gombojav O Wang Xi Murawski Robert K Sautenkov Vladimir A Sokolov Alexei V Scully Marlan O |
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Institution: | Department of Physics, Texas A&M University, College Station, TX 77843, USA. dmip@neo.tamu.edu |
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Abstract: | 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. |
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