Application of a time-dependent Hartree approach on several surfaces to the vibrational predissociation of Ne2I2

In this work we explore the application of a time-dependent Hartree (TDH) scheme to study the vibrational predissociation of Ne₂I₂ van der Waals clusters. The present approach is based on equations of motion extracted from the usual variational principle where the Hamiltonian has been previously represented in a set of diatomic vibrational states. The procedure leads to a set of coupled equations for the different modes on each diabatic state with, however, explicit separation between those modes. The application on a problem that inherently requires longtime propagation is shown to be successful. Calculated lifetimes compare well with previous calculations as well as with available experimental data. A more detailed mechanism, as the breath of the angular mode on the different vibrational channels, is better described.