Supplementary Material Available:Tables of diffusion coefficient D, spectral variance V, and T / q (q being the solvent viscosity) for polystyrene sphere probes in water, water:erythritol, water:glycerol, and pure glycerol; figures showing D and Vagainst TI,, (q being the solvent viscosity) for polystyrene sphere probes in water, watererythritol, and water:glycerol solutions (36 pages). Ordering information is given on any current masthead page.We investigate the process of internal rotational predissociation in the NeHF and NeDF van der Waals complexes using time-dependent quantum mechanical calculations. The computations are performed in three degrees of freedom and for arbitrary values of the total angular momentum; they use a combination of the Fourier wave packet propagation method in the dissociative coordinate with a body-fixed basis set expansion in the intramolecular angular coordinates. Calculated values of the predissociation lifetimes of several states of these complexes are found to be in excellent agreement with the results of time-independent quantum calculations. Product distributions are easily extracted from the evolving wave packets.The fragmentation mechanisms of several metastable states are further explored by examination of the time-evolving probability distribution.

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