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There has been much discussion (see refs. [37,38] and references therein, and [39] for an original reference) in the literature on the applicability of Bloch equations (the dynamic NMR-like interpretation) to dynamic vibrational band coalescence, and if they do reproduce experimental results, what the ultimate interpretation should be and whether the characteristic "lifetimes" determined from simulation should have a physical interpretation. One conclusion to draw from much of this discussion is that a detailed knowledge of the specific vibrational and "reaction" dynamics of each particular system (including knowledge of the formation of a low-energy transition state) is required for meaningful interpretation of vibrational band shapes, and for this reason accurate density functional or ab initio calculations on molecular systems of interest can be indispensable. See reference [16] for an example of such a study.
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