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arXiv:2203.13598 · Physical Review Letters

Symmetry Breaking in Sticky Collisions between Ultracold Molecules

Marijn P. Man, Gerrit C. Groenenboom, Tijs Karman

Published Dec 6, 2022• 9 citations
arXivHTMLPDF

Abstract

Ultracold molecules undergo "sticky collisions" that result in loss even for chemically nonreactive molecules. Sticking times can be enhanced by orders of magnitude by interactions that lead to nonconservation of nuclear spin or total angular momentum. We present a quantitative theory of the required strength of such symmetry-breaking interactions based on classical simulation of collision complexes. We find static electric fields as small as 10 V/cm can lead to nonconservation of angular momentum, while we find nuclear spin is conserved during collisions. We also compute loss of collision complexes due to spontaneous emission and absorption of black-body radiation, which are found to be slow.

DOI
10.1103/physrevlett.129.243401

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Ultracold molecules undergo "sticky collisions" that result in loss even for chemically nonreactive molecules. Sticking times can be enhanced by orders of magnitude by interactions that lead to nonconservation of nuclear spin or total angular momentum. We present a quantitative theory of the required strength of such symmetry-breaking interactions based on classical simulation of collision complexes. We find static electric fields as small as 10 V/cm can lead to nonconservation of angular momentum, while we find nuclear spin is conserved during collisions. We also compute loss of collision complexes due to spontaneous emission and absorption of black-body radiation, which are found to be slow.
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.
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.
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.
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.
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.
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.