4. Ultrafast Vibrational Relaxation in Unique Molecular Solids (e.g. with large vibrational energy gaps)

Energy Bottlenecks yield Very Long Vibrational Relaxation - and multi-phonon relaxation mechanisms

4a. picosecond CARS measurements of vibrational dynamics in uranyl crystals

4b. a large energy gap below the symmetric uranium oxygen stretch precludes simple fission decay.

4c. 5th and 6th order decay mechanisms result in a very long relaxation time (i.e decay rate drops exponentially with the order).

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