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.

arXiv comment7 pages, 4 figures, 1 table, submitted to Journal of Quantitative Spectroscopy and Radiative Transfer

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• Very accurate time propagation of coupled Schrödinger equations for femto- and attosecond physics and chemistry, with C++ source code