Fragment momentum distributions obtained from coupled electron-nuclear dynamics

J Chem Phys. 2012 Mar 14;136(10):104306. doi: 10.1063/1.3691831.

Abstract

We theoretically investigate fragmentation processes induced by femtosecond laser pulses within a model which incorporates electronic and nuclear motion. Single-pulse excitation leads to diffraction patterns in the electron momentum distribution which depend on the nature of the electronic state and also on the nuclear charge distribution. Additional structures appear in the nuclear momentum distribution if two time-delayed pulses produce fragments in the same dissociation channel. It is shown that these functions are modified by the electronic degree-of-freedom. A simultaneous excitation of two different electronic states results in further interferences which are related to electronic wave-packet dynamics on the attosecond time-scale.