Abstract The fundamental aspects of excited dynamics in polyatomic molecules contains many effects, which while understood in the limit of a sparse density of states in a simple diatomic, have long eluded study. With a combination of lasers, supersonic beams to prepare ultra-cold molecules and novel types of spectroscopic approaches, one can begin to observe the dynamics and properties of superposition states which are the basis of phenomena ranging from autoionization, to predissociation, to quantum interference effects and intramolecular vibrational redistribution. This paper will review selected studies on large polyatomic molecules and their clusters.

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