Abstract
The first experimental observation of sequential decay of metastable molecular cluster ions is reported. N 2 cluster ions are produced by electron impact ionization of a supersonic N 2 cluster beam and analyzed by a double-focusing sector field mass spectrometer (reversed geometry). It is found that metastable N 2 cluster ions lose more than one N 2 molecule in the microsecond time regime and decay predominantly via sequential series (N 2) n +* → (N 2) n-1 +* → … → N 2 +, evaporating a single monomer in each of these successive decay steps. The metastable decay rates determined in detail for cluster sizes 2 ⩽ n ⩽ 6 and n = 20 lie between 1 and 10 6 s −1 and depend strongly on the time elapsed after ion formation. The decay rates exhibit a quasi-periodic pattern, consistent with the assumption that up to four vibrational quanta (stored in neutral N 2 molecules within the cluster) relax into the phonon bath of the cluster during the sampling time.
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