Three-dimensional momentum imaging of dissociation in flight of metastable molecules

Abstract

We investigate dissociation in flight of metastable molecular dications formed by ultrashort, intense laser pulses using the cold target recoil ion momentum spectroscopy technique. A method for retrieving the lifetime(s) of the transient metastable state(s) as well as the complete three-dimensional momenta of the dissociating fragments is presented. Specifically, we demonstrate and discuss this approach by focusing on dissociation in flight of the ethylene dication going to the deprotonation channel. Two lifetimes are found to be associated with this process, C2H${}_{4}^{2+},\to $ C2H3 + + H+: τ1=202±10 ns and τ2=916±40 ns. For the corresponding channel in deuterated ethylene, lifetimes of τ1=269±29 ns and τ2=956±83 ns are obtained.