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