Optimization of the Femtosecond Laser Impulse for Excitation and the Spin-Orbit Mediated Dissociation in the NaRb Dimer

Abstract: We study the dynamics of multiple coupled states under the influence of an arbitrary time-dependent external field to investigate the femtosecond laser-driven excitation and the spin-orbit mediated dissociation in the NaRb dimer. In this process, the dimer is excited from the ground triplet state $1^3\Sigma^+$ to the $1^3\Pi$ state using the femtosecond laser impulse and the spin-orbit coupling between the $1^3\Pi$ and $2^1\Sigma^+$ states results in the singlet-triplet transition. The laser impulse parameters are optimised to obtain maximum yield in electronic states correlating with the first excited atomic asymptote. We observe the detailed population statistics and power-law decay of these states. Finally, the analysis of the population oscillations allows us to determine the optimal time delay for dumping the molecule to its absolute ground state.