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Journal of Quantitative Spectroscopy and Radiative Transfer

Electronic energy transfer in a dense level system

C. Gabbanini, M. Biagini, Silvia Gozzini, A. Lucchesini, A. Kopystyńska, L. Moi

Published Feb 1, 1992• 4 citations
Publisher
DOI
10.1016/0022-4073(92)90068-f

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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.
A formalism based on the generalized Langevin equation is used to obtain the dynamic response \ensuremath{\chi}(k,\ensuremath{\omega}) and relaxation function \ensuremath{\Xi}(k,t) of a dense electron gas in spatial dimension D for the low-momentum-transfer regime k\ensuremath{\ll}kF{\mathit{k}}_{\mathit{F}}kF​. Our results agree with known results for D=1, 2, and 3. In one dimension, the relaxation process is purely oscillatory. For D=4, we find a temporal scaling behavior, i.e., self-similarity of relaxation functions at different hierarchy levels. And in infinite dimensions, the system shows a Gaussian relaxation. The formalism is also extended to apply to an interacting system.