Stimulating the production of deeply bound RbCs molecules with laser pulses: the role of spin-orbit coupling in forming ultracold molecules

TL;DR

This study explores how laser pulses can efficiently produce deeply bound ultracold RbCs molecules, emphasizing the influence of spin-orbit coupling and contrasting heteronuclear with homonuclear systems.

Contribution

It provides a detailed analysis of the quantum dynamics and spin-orbit effects in forming ultracold RbCs molecules via two-color photoassociation, highlighting differences from Rb_2.

Findings

RbCs wavepackets reach short-range in 13 ps, faster than Rb_2.

Significant probability of forming ground-state molecules up to 1500 cm-1 binding energy.

Spin-orbit coupling influences the character of excited states and deexcitation pathways.

Abstract

We investigate the possibility of forming deeply bound ultracold RbCs molecules by a two-color photoassociation experiment. We compare the results with those for Rb_2 in order to understand the characteristic differences between heteronuclear and homonuclear molecules. The major differences arise from the different long-range potential for excited states. Ultracold 85Rb and 133Cs atoms colliding on the X^1Sigma+ potential curve are initially photoassociated to form excited RbCs molecules in the region below the Rb(5S) + Cs(6P_1/2) asymptote. We explore the nature of the Omega=0^+ levels in this region, which have mixed A^1Sigma^+ and b^3Pi character. We then study the quantum dynamics of RbCs by a time-dependent wavepacket (TDWP) approach. A wavepacket is formed by exciting a few vibronic levels and is allowed to propagate on the coupled electronic potential energy curves. For a detuning of 7.5 cm-1, the wavepacket for RbCs reaches the short-range region in about 13 ps, which is significantly faster than for the homonuclear Rb_2 system; this is mostly because of the absence of an R^-3 long-range tail in the excited-state potential curves for heteronuclear systems. We give a simple semiclassical formula that relates the time taken to the long-range potential parameters. For RbCs, in contrast to Rb_2, the excited-state wavepacket shows a substantial peak in singlet density near the inner turning point, and this produces a significant probability of deexcitation to form ground-state molecules bound by up to 1500 cm-1. Our analysis of the role of spin-orbit coupling concerns the character of the mixed states in general and is important for both photoassociation and stimulated Raman deexcitation.