Abstract
The first experimental observation of sequential decay of metastable cluster ions is reported herein. Ar cluster ions are produced by electron-impact ionization of a supersonic Ar cluster beam. Some of these ions are observed to decay via sequential decay series in the microsecond time scale, i.e., Arn+*Arn1+*Arn2+* (with n≥7), evaporating a single monomer in each of these successive decays. Conversely, the dominant metastable decay of Ar4 +*Ar2 + proceeds predominantly via a single-step fissioning process leading to the simultaneous evaporation of two neutral Ar monomers.