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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 t rapped 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 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 explore the properties of 3-atom complexes of alkali-metal diatomic molecules with alkali-metal atoms, which may be formed in ultracold collisions. We estimate the densities of vibrational states at the energy of atom-diatom collisions, and find v alues ranging from 2.2 to 350~K$^{-1}$. However, this density does not account for electronic near-degeneracy or electron and nuclear spins. We consider the fine and hyperfine structure expected for such complexes. The Fermi contact interaction between electron and nuclear spins can cause spin exchange between atomic and molecular spins. It can drive inelastic collisions, with resonances of three distinct types, each with a characteristic width and peak height in the inelastic rate coefficient. Some of these resonances are broad enough to overlap and produce a background loss rate that is approximately proportional to the number of outgoing inelastic channels. Spin exchange can increase the density of states from which laser-induced loss may occur.
We present measurements of more than 80 magnetic Feshbach resonances in collisions of ultracold $^{23}$Na$^{40}$K with $^{40}$K. We assign quantum numbers to a group of low-field resonances and show that they are due to long-range states of the triat omic complex in which the quantum numbers of the separated atom and molecule are approximately preserved. The resonant states are not members of chaotic bath of short-range states. Similar resonances are expected to be a common feature of alkali-metal diatom + atom systems.
Polar molecules are an emerging platform for quantum technologies based on their long-range electric dipole-dipole interactions, which open new possibilities for quantum information processing and the quantum simulation of strongly correlated systems . Here, we use magnetic and microwave fields to design a fast entangling gate with $>0.999$ fidelity and which is robust with respect to fluctuations in the trapping and control fields and to small thermal excitations. These results establish the feasibility to build a scalable quantum processor with a broad range of molecular species in optical-lattice and optical-tweezers setups.
Characterizing quasibound states from coupled-channel scattering calculations can be a laborious task, involving extensive manual iteration and fitting. We present an automated procedure, based on the phase shift or S-matrix eigenphase sum, that reli ably converges on a quasibound state (or scattering resonance) from some distance away. It may be used for both single-channel and multichannel scattering. It produces the energy and width of the state and the phase shift of the background scattering, and hence the lifetime of the state. It also allows extraction of partial widths for decay to individual open channels. We demonstrate the method on a very narrow state in the Van der Waals complex Ar--H$_2$, which decays only by vibrational predissociation, and on near-threshold states of $^{85}$Rb$_2$, whose lifetime varies over 4 orders of magnitude as a function of magnetic field.
We have investigated Feshbach resonances in collisions of high-spin atoms such as Er and Dy with closed-shell atoms such as Sr and Yb, using coupled-channel scattering and bound-state calculations. We consider both low-anisotropy and high-anisotropy limits. In both regimes we find many resonances with a wide variety of widths. The wider resonances are suitable for tuning interatomic interactions, while some of the narrower resonances are highly suitable for magnetoassociation to form high-spin molecules. These molecules might be transferred to short-range states, where they would have large magnetic moments and electric dipole moments that can be induced with very low electric fields. The results offer the opportunity to study mixed quantum gases where one species is dipolar and the other is not, and open up important prospects for a new field of ultracold high-spin polar molecules.
We study the behavior of the Eisenbud-Wigner collisional time delay around Feshbach resonances in cold and ultracold atomic and molecular collisions. We carry out coupled-channels scattering calculations on ultracold Rb and Cs collisions. In the low- energy limit, the time delay is proportional to the scattering length, so exhibits a pole as a function of applied field. At high energy, it exhibits a Lorentzian peak as a function of either energy or field. For narrow resonances, the crossover between these two regimes occurs at an energy proportional to the square of the resonance strength parameter $s_textrm{res}$. For wider resonances, the behavior is more complicated and we present an analysis in terms of multichannel quantum defect theory.
We investigate magnetically tunable Feshbach resonances in ultracold collisions between ground-state Yb and Cs atoms, using coupled-channel calculations based on an interaction potential recently determined from photoassociation spectroscopy. We pred ict resonance positions and widths for all stable isotopes of Yb, together with resonance decay parameters where appropriate. The resonance patterns are richer and more complicated for fermionic Yb than for spin-zero isotopes, because there are additional level splittings and couplings due to scalar and tensorial Yb hyperfine interactions. We examine collisions involving Cs atoms in a variety of hyperfine states, and identify resonances that appear most promising for experimental observation and for magnetoassociation to form ultracold CsYb molecules.
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 RbCs 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 study the two-body bound states of a model Hamiltonian that describes the interaction between two field-oriented dipole moments. This model has been used extensively in many-body physics of ultracold polar molecules and magnetic atoms, but its few -body physics has been explored less fully. With a hard-wall short-range boundary condition, the dipole-dipole bound states are universal and exhibit a complicated pattern of avoided crossings between states of different character. For more realistic Lennard-Jones short-range interactions, we consider parameters representative of magnetic atoms and polar molecules. For magnetic atoms, the bound states are dominated by the Lennard-Jones potential, and the perturbative dipole-dipole interaction is suppressed by the special structure of van der Waals bound states. For polar molecules, we find a dense manifold of dipole-dipole bound states with many avoided crossings as a function of induced dipole or applied field, similar to those for hard-wall boundary conditions. This universal pattern of states may be observable spectroscopically for pairs of ultracold polar molecules.
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