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arXiv:2103.00889 · Physical Review Research

Collisions of ultracold molecules in bright and dark optical dipole traps

Roman Bause, Andreas Schindewolf, Renhao Tao, Marcel Duda, Xing-Yan Chen, Goulven Quéméner, Tijs Karman, Arthur Christianen, Immanuel Bloch, Xin-Yu Luo

Published Jul 2, 2021• 89 citations
arXivHTMLPDF

Abstract

Understanding collisions between ultracold molecules is crucial for making stable molecular quantum gases and harnessing their rich internal degrees of freedom for quantum engineering. Transient complexes can strongly influence collisional physics, but in the ultracold regime, key aspects of their behavior have remained unknown. To explain experimentally observed loss of ground-state molecules from optical dipole traps, it was recently proposed that molecular complexes can be lost due to photoexcitation. By trapping molecules in a repulsive box potential using laser light near a narrow molecular transition, we are able to test this hypothesis with light intensities three orders of magnitude lower than what is typical in red-detuned dipole traps. This allows us to investigate light-induced collisional loss in a gas of nonreactive fermionic $^{23}\mathrm{Na}^{40}\mathrm{K}$ molecules. Even for the lowest intensities available in our experiment, our results are consistent with universal loss, meaning unit loss probability inside the short-range interaction potential. Our findings disagree by at least two orders of magnitude with latest theoretical predictions, showing that crucial aspects of molecular collisions are not yet understood and provide a benchmark for the development of new theories.

DOI
10.1103/physrevresearch.3.033013

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Understanding collisions between ultracold molecules is crucial for making stable molecular quantum gases and harnessing their rich internal degrees of freedom for quantum engineering. Transient complexes can strongly influence collisional physics, but in the ultracold regime, key aspects of their behavior have remained unknown. To explain experimentally observed loss of ground-state molecules from optical dipole traps, it was recently proposed that molecular complexes can be lost due to photoexcitation. By trapping molecules in a repulsive box potential using laser light near a narrow molecular transition, we are able to test this hypothesis with light intensities three orders of magnitude lower than what is typical in red-detuned dipole traps. This allows us to investigate light-induced collisional loss in a gas of nonreactive fermionic 23Na40K^{23}\mathrm{Na}^{40}\mathrm{K}23Na40K molecules. Even for the lowest intensities available in our experiment, our results are consistent with universal loss, meaning unit loss probability inside the short-range interaction potential. Our findings disagree by at least two orders of magnitude with latest theoretical predictions, showing that crucial aspects of molecular collisions are not yet understood and provide a benchmark for the development of new theories.
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Measurements of the temperature dependence of trap loss collisions of laser-cooled rubidium atoms are presented. A significant suppression of the rate of collisions between ground- and excited-state atoms is observed for temperatures below $\\sim$70 mu\\mumuK. In such inelastic collisions, the atomic excitation takes place at long range and must survive against spontaneous decay to short range. Our results are consistent with recent predictions for the low temperature suppression of these collisions due to reduced survival of atomic excitation at low collision velocities.^ We report on measurements of trap loss collisions between ultracold Rb atoms which are confined in a magneto-optical trap. Both isotopes sp85\\sp{85}sp85Rb and sp87\\sp{87}sp87Rb have been studied over wide range of trap laser intensities and detunings. The trap loss collision rates exhibit variations over 3 orders of magnitude. We observe significant differences between the isotopes. At large detunings the ability of the trap to recapture products of the hyperfine-changing collisions is significantly diminished. This finding is supported by our numerical simulations of the recapture process. The trap loss rates due to collisions with room temperature background gas have also been measured.^ Using laser light tuned to a repulsive molecular potential, we have been able to suppress inelastic ground-state hyperfine changing collisions between ultracold sp87\\sp{87}sp87Rb atoms. Adiabatic excitation to the repulsive curve alters the atomic trajectories and prevents the atoms from approaching close enough for the hyperfine change to occur. Experimental results show suppressions up to $\\sim$50% and are in reasonable agreement with a simple Landau-Zener model.^ Finally, we have observed a significant cooperative effect in ultracold trap loss collisions induced by two separate lasers. One laser, tuned close to the atomic resonance, excites the atom pair to an attractive potential at long range. The resulting acceleration and deflection give rise to an enhancement in the collisional flux of ground-state atoms reaching short range, as probed by a second laser. Enhancements up to a factor of $\\sim$3 have been observed. ^
Abstract Understanding ultracold collisions involving molecules is of fundamental importance for current experiments, where inelastic collisions typically limit the lifetime of molecular ensembles in optical traps. Here we present a broad study of optically trapped ultracold RbCs molecules in collisions with one another, in reactive collisions with Rb atoms, and in nonreactive collisions with Cs atoms. For experiments with RbCs alone, we show that by modulating the intensity of the optical trap, such that the molecules spend 75% of each modulation cycle in the dark, we partially suppress collisional loss of the molecules. This is evidence for optical excitation of molecule pairs mediated via sticky collisions. We find that the suppression is less effective for molecules not prepared in the spin-stretched hyperfine ground state. This may be due either to longer lifetimes for complexes in the dark or to laser-free decay pathways. For atom–molecule mixtures, RbCs + Rb and RbCs + Cs, we demonstrate that the rate of collisional loss of molecules scales linearly with the density of atoms. This indicates that, in both cases, the loss of molecules is rate-limited by two-body atom–molecule processes. For both mixtures, we measure loss rates that are below the thermally averaged universal limit.
Collisional complexes, which are formed as intermediate states in molecular collisions, are typically short-lived and decay within picoseconds. However, in ultracold collisions involving bialkali molecules, complexes can live for milliseconds, completely changing the collision dynamics. This can lead to unexpected two-body loss in samples of nonreactive molecules. During the past decade, such "sticky" collisions have been a major hindrance in the preparation of dense and stable molecular samples, especially in the quantum-degenerate regime. Currently, the behavior of the complexes is not fully understood. For example, in some cases, their lifetime has been measured to be many orders of magnitude longer than recent models predict. This is not only an intriguing problem in itself but also practically relevant, since understanding molecular complexes may help to mitigate their detrimental effects. Here, we review the recent experimental and theoretical progress in this field. We treat the case of molecule-molecule as well as molecule-atom collisions.
The lifetime of nonreactive ultracold bialkali gases was conjectured to be limited by sticky collisions amplifying three-body loss. We show that the sticking times were previously overestimated and do not support this hypothesis. We find that electronic excitation of NaK+NaK collision complexes by the trapping laser leads to the experimentally observed two-body loss. We calculate the excitation rate with a quasiclassical, statistical model employing ab initio potentials and transition dipole moments. Using longer laser wavelengths or repulsive box potentials may suppress the losses.
Recent experiments on ultracold nonreactive dipolar molecules have observed high two-body losses, even though these molecules can undergo neither inelastic, nor reactive (as they are in their absolute ground state), nor light-assisted collisions (if they are measured in the dark). In the presence of an electric field these losses seem to be near universal (the probability of loss at short range is near unity) while in the absence of it the losses seem nonuniversal. To explain these observations we propose a simple model based on the mixing effect of an electric field on the states of the two diatomic molecules at long range and on the density of states of the tetramer complex formed at short range, believed to be responsible for the losses. We apply our model to collisions of ground-state molecules of endothermic systems, of current experimental interest.