title: Coherent versus incoherent Raman scattering: molecular coherence excitation and measurement.
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.
authors.affiliation: Department of Physics, Texas A&M University, College Station, TX 77843, USA. dmip@neo.tamu.edu
authors.forename: Dmitry
authors.initials: D
authors.lastname: Pestov
authors.forename: Gombojav O
authors.initials: GO
authors.lastname: Ariunbold
authors.forename: Xi
authors.initials: X
authors.lastname: Wang
authors.forename: Robert K
authors.initials: RK
authors.lastname: Murawski
authors.forename: Vladimir A
authors.initials: VA
authors.lastname: Sautenkov
authors.forename: Alexei V
authors.initials: AV
authors.lastname: Sokolov
authors.forename: Marlan O
authors.initials: MO
authors.lastname: Scully