The unimolecular decomposition of single ethylene ions in association with argon clusters containing more than 100 atoms has been observed. Fragmentation on these large clusters provides strong support for the proposal that a charge-transfer mechanism is responsible for exciting the molecular ions. In addition, the results show evidence of enhanced fragmentation for those molecular ions associated with a “magic number” of inert gas atoms. From these observations it is suggested that reactant ions lie on, or close to, the surface of a cluster.
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