Abstract
We investigated the nuclear dynamics of diatomic molecular ions in intense laser fields by analyzing their fragment kinetic-energy release (KER) spectra as a function of the pump-probe delay $\ensuremath{\tau}$. Within the Born-Oppenheimer (BO) approximation, we calculated ab initio adiabatic potential-energy curves and their electric dipole couplings, using the quantum chemistry code gamess. By comparing simulated KER spectra as a function of either $\ensuremath{\tau}$ or the vibrational quantum-beat frequency for the nuclear dynamics on both individual and dipole-coupled BO potential curves with measured spectra, we developed a scheme for identifying electronic states that are relevant for the dissociation dynamics. We applied this scheme to investigate the nuclear dynamics in O${}_{2}$${}^{+}$ ions that are produced by ionization of neutral O${}_{2}$ molecules in an ultrashort infrared (IR) pump pulse and dissociate due to the dipole coupling of molecular potential curves in a delayed IR probe laser field.
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