The authors study the structure of four-atom complexes which can be formed in collisions of ultracold molecules, demonstrating that couplings between internal states can be large enough to increase their lifetime beyond semiclassical estimates. They consider the interplay between the complex lifetime, photon absorption rate from the trapping laser, and secondary inelastic collisions with the remaining molecules and show that it can lead to vastly different scenarios of the loss dynamics.
The authors study the structure of four-atom complexes which can be formed in collisions of ultracold molecules, demonstrating that couplings between internal states can be large enough to increase their lifetime beyond semiclassical estimates. They consider the interplay between the complex lifetime, photon absorption rate from the trapping laser, and secondary inelastic collisions with the remaining molecules and show that it can lead to vastly different scenarios of the loss dynamics.
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.
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.
We study collisions in an optically trapped, pure sample of ultracold Cs 2 molecules in various internal states. The molecular gas is created by Feshbach association from a near-degenerate atomic gas, with adjustable temperatures in the nanokelvin range. We identify several narrow loss resonances, which point to the coupling to more complex molecular states and may be interpreted as Feshbach resonances in dimerdimer interactions. Moreover, in some molecular states we observe a surprising temperature dependence in collisional loss. This shows that the situation cannot be understood in terms of the usual simple threshold behavior for inelastic two-body collisions. We interpret this observation as further evidence for a more complex molecular structure beyond the well-understood dimer physics.
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.
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 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.
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.