Optimization of the Femtosecond Laser Impulse for Photoassociation and the Power-Law Decay for the Spin-Orbit Mediated Dissociation in the NaRb Dimer

We use our newly-developed quantum dynamics code that allows us to study the dynamics of multiple coupled states under the influence of an arbitrary time-dependent external field, to investigate the femtosecond laser-driven process of association and the forbidden transition 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 pulse and next, the spin-orbit coupling between the $1^3\Pi$ and $2^1\Sigma^+$ states results in the singlet-triplet transition. The laser pulse parameters are optimised to obtain maximum yield in electronic levels 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 for the determination of the optimal time delay for dumping molecule to its absolute ground state.