We have performed time-resolved studies of the dynamics of thermal isomerization occurring in certain cesium-halide cluster anions. Using a pump-probe technique, we have observed the repopulation of a photodepleted isomer within an ensemble as a function of time by monitoring the photoelectron spectrum. The rates of isomerization increase and the isomer lifetimes decrease as functions of temperature. The clusters undergo a gradual phase transition from solidlike to liquidlike states with liquidlike behavior obtained at ~500 K, much lower than the bulk melting temperatures of ~900 K.
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