Population and phase relaxation in two molecular models is studied. The analysis is based on recent work by Lindblad, in which the time evolution of an N-level quantum system is described using the coresponding generator of a completely positive semigroup. One of the models studied corresponds to a diatomic molecule in a dense medium. New results are obtained for the influence of two quantum transitions on population and phase relaxation. The other model studied corresponds to the case of exchange dephasing in a polyatomic molecule embedded in a dense medium. The formalism permits inclusion of coupling terms neglected by Harris, Shelby, and Cornelius; it is shown that inclusion of these terms leads to a rich range of line shapes, which information is not available from the approximation used by Harris et al.
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Kosloff et al. (1980) studied this question.
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