Geometrical and statistical factors in fission of small metal clusters

Abstract

Fission of metastable charged univalent metal clusters has been studied on example of Na_{10}^{2+} and Na_{18}^{2+} clusters by means of density functional theory methods. Energetics of the process, i.e. dissociation energies and fission barriers, as well as its dynamics, i.e. fission pathways, have been analyzed. The dissociation energies and fission barriers have been calculated for the full range of fission channels for the Na_{10}^{2+} cluster. The impact of cluster structure on the fission process has been elucidated. The calculations show that the geometry of the smaller fragment and geometry of its immediate neighborhood in the larger fragment play a leading role in defining the fission barrier height. The present study demonstrates importance of rearrangement of the cluster structure during fission. It may include forming a neck between the two fragments or fissioning via another isomer state of the parent cluster; examples of such processes are given. For several low-lying isomers of Na_{10}^{2+} cluster the potential barriers for transitions between these isomer states are calculated and compared with the corresponding fission barriers. These data suggest that there is a competition between "direct" fission and fission going via intermediate isomer states of the parent cluster. An impact of the cluster geometry on the change of the system's entropy due to fission is also discussed.