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Energy and phase relaxation accompanying impulsive reactions in liquids

Experiments made possible by new laser methods explore ultrafast features of solution phase reaction dynamics. The results from two examples are given. Photodissociation of small molecules such as and in solution yields highly excited vibrational state distributions and narrow bond length distributions. The dynamics in the transition state region and the ensuing dynamics can be followed by femtosecond laser experiments that probe the phase and energy loss processes. The mercuric iodide experiments show that the phase relaxation is dominated by coherence transfer processes which have a strong analogy to classical motions. The population relaxation dynamics gives results similar to those from classical molecular dynamics simulations which suggest, notwithstanding the significant polarity of the molecules and solvents, that the relaxations are dominated by Lennard - Jones repulsion at sufficiently low frequencies.