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arXiv:2109.08016 · New Journal of Physics

Molecule–molecule and atom–molecule collisions with ultracold RbCs molecules

Philip D. Gregory, Jacob A. Blackmore, Matthew D. Frye, Luke Fernley, Sarah Bromley, Jeremy M. Hutson, Simon L. Cornish

Published Nov 23, 2021• 3 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1088/1367-2630/ac3c63

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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.
Abstract Understanding and controlling collisions is crucial to the burgeoning field of ultracold molecules. All experiments so far have observed fast loss of molecules from the trap. However, the dominant mechanism for collisional loss is not well understood when there are no allowed 2-body loss processes. Here we experimentally investigate collisional losses of nonreactive ultracold 87 Rb 133 Cs molecules, and compare our findings with the sticky collision hypothesis that pairs of molecules form long-lived collision complexes. We demonstrate that loss of molecules occupying their rotational and hyperfine ground state is best described by second-order rate equations, consistent with the expectation for complex-mediated collisions, but that the rate is lower than the limit of universal loss. The loss is insensitive to magnetic field but increases for excited rotational states. We demonstrate that dipolar effects lead to significantly faster loss for an incoherent mixture of rotational states.
We show that the lifetime of ultracold ground-state ^{87}Rb^{133}Cs molecules in an optical trap is limited by fast optical excitation of long-lived two-body collision complexes. We partially suppress this loss mechanism by applying square-wave modulation to the trap intensity, such that the molecules spend 75% of each modulation cycle in the dark. By varying the modulation frequency, we show that the lifetime of the collision complex is 0.53±0.06 ms in the dark. We find that the rate of optical excitation of the collision complex is 3_{-2}^{+4}×10^{3} W^{-1} cm^{2} s^{-1} for λ=1550 nm, leading to a lifetime of <100 ns for typical trap intensities. These results explain the two-body loss observed in experiments on nonreactive bialkali molecules.
Abstract Understanding and controlling collisions is crucial to the burgeoning field of ultracold molecules. All experiments so far have observed fast loss of molecules from the trap. However, the dominant mechanism for collisional loss is not well understood when there are no allowed 2-body loss processes. Here we experimentally investigate collisional losses of nonreactive ultracold 87Rb133Cs molecules, and compare our findings with the sticky collision hypothesis that pairs of molecules form long-lived collision complexes. We demonstrate that loss of molecules occupying their rotational and hyperfine ground state is best described by second-order rate equations, consistent with the expectation for complex-mediated collisions, but that the rate is lower than the limit of universal loss. The loss is insensitive to magnetic field but increases for excited rotational states. We demonstrate that dipolar effects lead to significantly faster loss for an incoherent mixture of rotational states.
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. ^
A thorough understanding of molecular scattering in the ultralow temperature regime is crucial for realizing long coherence times and enabling tunable interactions in molecular gases, systems which offer many opportunities in quantum simulation, quantum information, and precision measurement.Of particular importance is the nature of the long-lived intermediate complexes which may be formed in ultracold molecular collisions, as such complexes can dramatically affect the stability of molecular gases, even when exothermic reaction channels are not present.Here, we investigate collisional loss in an ultracold mixture of 40 K 87 Rb molecules and 87 Rb atoms, where chemical reactions between the two species are energetically forbidden.Through direct detection of the KRb 2 Ã intermediate complexes formed from atom-molecule collisions, we show that a 1064 nm laser source used for optical trapping of the sample can efficiently deplete the complex population via photoexcitation, an effect which can explain the strong twobody loss observed in the mixture.By monitoring the time evolution of the KRb 2 Ã population after a sudden reduction in the 1064 nm laser intensity, we measure the lifetime of the complex [0.39(6) ms], as well as the photoexcitation rate for 1064 nm light [0.50ð3Þμs -1 ðkW=cm 2 Þ -1 ].The observed lifetime, which is ∼10 5 times longer than recent estimates based on the Rice-Ramsperger-Kassel-Marcus statistical theory, calls for new theoretical insight to explain its origin.
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.