SURFACE-HOPPING TRAJECTORY CALCULATIONS OF COLLISION-INDUCED DISSOCIATION PROCESSES WITH AND WITHOUT CHARGE-TRANSFER

Reaction cross sections for collision-induced dissociation (CID) Ne + He2+ → Ne + He + He+, collision-induced predissociation (CIP) Ne + He2+ → Ne+ + He + He, and ion-transfer (IT) Ne + He2+ → NeHe+ + He were computed from surface-hopping trajectories on a model diatomics-in-molecules potential surface for He2+ vibrational energies of 0.2, 0.8 and 1.7 eV and total collision energies of 2.7, 6.0 and 10.7 eV. In agreement with experiment, CIP is the dominant process at all energies; the calculations predict that its cross section has a maximum with respect to variation of the He2+ vibrational energy. CID is a small-impact parameter process giving rise to wider scattering angles than CIP. The IT reaction has a very small cross section at all energies. These results agree well with existing experiments and suggest new experiments with state-selected He2+ vibrational energy. The dynamics of reaction are interpreted in terms of a charge-transfer spectator model. © 1979.