Optimization of the femtosecond laser impulse for excitation and the spin-orbit-mediated dissociation in the NaRb molecule

High accuracy ab initio potential energy curves (1tSigma+, 2sSigma+, 1tPi), electronic transition dipole moment function (1tSigma+ - 1tPi), and spin-orbit coupling (2sSigma+ - 1tPi) have been calculated for the NaRb molecule. The time-dependent excitation and dissociation processes in the polar alkali diatomic NaRb molecule and the quantum properties of these reactions in their characteristic time regimes have been described. Optimizing of the femtosecond laser impulse parameters provides the transition from the 1tSigma+ state and maximization of the population in the coupled complex of excited electronic states (2sSigma+ - 1tPi) have been presented. Quantum dynamics simulations of the NaRb molecule in the coupled excited electronic states enabled the establishment of the optimal time delays for the femtosecond laser impulses in the association process enabling the formation of the cold molecules in the deeply bound ground state. The generally modified power-law decay allowed for the proper description of the spin-orbit-mediated dissociation process. All computations were performed using the MOLPRO program package and our newly-developed code for performing the quantum dynamics simulations.
The dataset contains six files whose contents are described in the NaRb_readme.txt file.