Complementary imaging of the nuclear dynamics in laser-excited diatomic molecular ions in the time and frequency domains

Abstract

Experimentally, the bound and dissociative nuclear dynamics in small molecular ions can be resolved in time by using intense ultrashort pump in combination with delayed probe laser pulses. We discuss the modelling of related pump–probe-delay-dependent fragment kinetic-energy-release (KER) spectra for the laser-induced dissociative ionization of selected diatomic molecules and show how the quantum-mechanical simulation of measured KER spectra—in both the time domain and as a function of the beat frequency between molecular vibrational levels—reveals dissociation pathways and the characteristics of initially occupied molecular potential curves.