Ion-induced molecular fragmentation: beyond the Coulomb explosion picture

Abstract

The fragmentation of the CO molecule by O⁷⁺ ion impact is investigated in two different energy regimes by fragment ion momentum spectroscopy. The improved resolution of the present kinetic energy release measurement together with application of a time-dependent wavepacket dynamics method used in conjunction with new high-level computations of a large number of dication potential energy curves enables one to unambiguously assign each line to an excited state of the transient molecular dication produced during the collision. This is the first direct experimental evidence of the limitations of the Coulomb explosion model to reproduce the molecular fragmentation dynamics induced by ion impact. Electron removal due to a capture process is shown to transfer less excitation to the target than direct ionization. At low collision velocity, the three-body interaction between the projectile and the two fragments is also clearly highlighted.