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Adiabatic transfer of population in a dense fluid: the role of dephasing statistics
Authors:Demirplak Mustafa  Rice Stuart A
Affiliation:Department of Chemistry, The University of Chicago, Chicago, Illinois 60637, USA.
Abstract:We report the results of simulation studies of the statistics of vibrational dephasing of a YCl (Y=H, D, T, and I) diatom in dense fluid Ar at two temperatures, including the effect of strong field driving on the energy level modulation statistics. The distribution of energy level modulations is found to be non-Gaussian with a high energy tail. Aspects of stimulated Raman adiabatic passage (STIRAP) between the vibrational levels of HCl in dense fluid Ar have been investigated. For HCl with nearly degenerate v=0-->v=1 and v=1-->v=2 transitions, the combined effect of modulation and power broadening reduces the STIRAP efficiency for population transfer from v=0 to v=2 of the order of 30%. However, if the transitions used have very different frequencies, as in the original model studied by Demirplak and Rice [J. Chem. Phys. 116, 8028 (2002)], the STIRAP efficiency for population transfer remains high, of the order of 80%, even with non-Gaussian modulation of energy levels.
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