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We prepare mixtures of ultracold CaF molecules and Rb atoms in a magnetic trap and study their inelastic collisions. When the atoms are prepared in the spin-stretched state and the molecules in the spin-stretched component of the first rotationally excited state, they collide inelastically with a rate coefficient of $k_2 = (6.6 \pm 1.5) \times 10^{-11}$ cm$^{3}$/s at temperatures near 100~$��$K. We attribute this to rotation-changing collisions. When the molecules are in the ground rotational state we see no inelastic loss and set an upper bound on the spin relaxation rate coefficient of $k_2 < 5.8 \times 10^{-12}$ cm$^{3}$/s with 95% confidence. We compare these measurements to the results of a single-channel loss model based on quantum defect theory. The comparison suggests a short-range loss parameter close to unity for rotationally excited molecules, but below 0.04 for molecules in the rotational ground state., 9 pages, 6 figures. Minor changes following review

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 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., Comment: 21 pages, 9 figures

We study three-atom inelastic scattering in ultracold ^{39}K near a Feshbach resonance of intermediate coupling strength. The nonuniversal character of such resonance leads to an abnormally large Efimov absolute length scale and a relatively small effective range r_{e}, allowing the features of the ^{39}K Efimov spectrum to be better isolated from the short-range physics. Meticulous characterization of and correction for finite-temperature effects ensure high accuracy on the measurements of these features at large-magnitude scattering lengths. For a single Feshbach resonance, we unambiguously locate four distinct features in the Efimov structure. Three of these features form ratios that obey the Efimov universal scaling to within 10%, while the fourth feature, occurring at a value of scattering length closest to r_{e}, instead deviates from the universal value.

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 reliably 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.

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., 13 pages, 5 figures

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 predict 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.

We investigate $\mathrm{Cs}+\mathrm{Cs}$ scattering in excited Zeeman and hyperfine states. We calculate the real and imaginary parts of the $s$-wave scattering length; the imaginary part directly provides the rate coefficient for two-body inelastic loss, while the real part allows us to identify regions of magnetic field where three-body recombination will be slow. We identify field regions where Cs in its $(f,{m}_{f})=(3,+2)$ and $(3,+1)$ states may be stable enough to allow Bose-Einstein condensation, and additional regions for these and the (3, 0) and $(3,\ensuremath{-}3)$ states where high-density clouds should be long-lived.

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 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., Comment: Accepted version

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 the 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.

We report the production of ultracold heteronuclear Cs$^*$Yb molecules through one-photon photoassociation applied to an ultracold atomic mixture of Cs and Yb confined in an optical dipole trap. We use trap-loss spectroscopy to detect molecular states below the Cs($^{2}P_{1/2}$) + Yb($^{1}S_{0}$) asymptote. For $^{133}$Cs$^{174}$Yb, we observe 13 rovibrational states with binding energies up to $\sim$500 GHz. For each rovibrational state we observe two resonances associated with the Cs hyperfine structure and show that the hyperfine splitting in the diatomic molecule decreases for more deeply bound states. In addition, we produce ultracold fermionic $^{133}$Cs$^{173}$Yb and bosonic $^{133}$Cs$^{172}$Yb and $^{133}$Cs$^{170}$Yb molecules. From mass scaling, we determine the number of bound states supported by the 2(1/2) excited-state potential to be 154 or 155., Comment: 9 Pages, 5 Figures

We perform two-photon photoassociation spectroscopy of the heteronuclear CsYb molecule to measure the binding energies of near-threshold vibrational levels of the $X~^{2}\Sigma_{1/2}^{+}$ molecular ground state. We report results for $^{133}$Cs$^{170}$Yb, $^{133}$Cs$^{173}$Yb and $^{133}$Cs$^{174}$Yb, in each case determining the energy of several vibrational levels including the least-bound state. We fit an interaction potential based on electronic structure calculations to the binding energies for all three isotopologs and find that the ground-state potential supports 77 vibrational levels. We use the fitted potential to predict the interspecies s-wave scattering lengths for all seven Cs+Yb isotopic mixtures., Comment: 11 pages, 8 figures, 4 tables

We describe procedures for converging on and characterizing zero-energy Feshbach resonances that appear in scattering lengths as a function of an external field. The elastic procedure is appropriate for purely elastic scattering, where the scattering length is real and displays a true pole. The regularized scattering length (RSL) procedure is appropriate when there is weak background inelasticity, so that the scattering length is complex and displays an oscillation rather than a pole, but the resonant scattering length $a_{\rm res}$ is close to real. The fully complex procedure is appropriate when there is substantial background inelasticity and the real and complex parts of $a_{\rm res}$ are required. We demonstrate these procedures for scattering of ultracold $^{85}$Rb in various initial states. All of them can converge on and provide full characterization of resonances, from initial guesses many thousands of widths away, using scattering calculations at only about 10 values of the external field., 9 pages, 5 figures

We present measurements of interspecies thermalization between ultracold samples of $^{133}$Cs and either $^{174}$Yb or $^{170}$Yb. The two species are trapped in a far-off-resonance optical dipole trap and $^{133}$Cs is sympathetically cooled by Yb. We extract effective interspecies thermalization cross sections by fitting the thermalization measurements to a rate equation model, giving $\sigma_{\mathrm{Cs^{174}Yb}} = \left(5 \pm 2\right) \times 10^{-13} \, \mathrm{cm^{2}}$ and $\sigma_{\mathrm{Cs^{170}Yb}} = \left(18 \pm 8\right) \times 10^{-13} \, \mathrm{cm^{2}}$. We perform quantum scattering calculations of the thermalization cross sections and optimize the CsYb interaction potential to reproduce the measurements. We predict scattering lengths for all isotopic combinations of Cs and Yb. We also demonstrate the independent production of $^{174}$Yb and $^{133}$Cs Bose-Einstein condensates using the same optical dipole trap, an important step towards the realization of a quantum-degenerate mixture of the two species., Comment: 12 pages, 7 figures

We calculate near-threshold bound states and Feshbach resonance positions for atom + rigid-rotor models of the highly anisotropic systems Li+CaH and Li+CaF. We perform statistical analysis on the resonance positions to compare with the predictions of random matrix theory. For Li+CaH with total angular momentum $J=0$ we find fully chaotic behavior in both the nearest-neighbor spacing distribution and the level number variance. However, for $J>0$ we find different behavior due to the presence of a nearly conserved quantum number. Li+CaF ($J=0$) also shows apparently reduced levels of chaotic behavior despite its stronger effective coupling. We suggest this may indicate the development of another good quantum number relating to a bending motion of the complex. However, continuously varying the rotational constant over a wide range shows unexpected structure in the degree of chaotic behavior, including a dramatic reduction around the rotational constant of CaF. This demonstrates the complexity of the relationship between coupling and chaotic behavior., 13 pages, 10 figures

We calculate and analyze Feshbach resonance spectra for ultracold $\mathrm{Yb}({}^{1}{S}_{0})+\mathrm{Yb}({}^{3}{P}_{2})$ collisions as a function of an interatomic potential scaling factor $\ensuremath{\lambda}$ and external magnetic field. We show that, at zero field, the resonances are distributed randomly in $\ensuremath{\lambda}$, but that signatures of quantum chaos emerge as a field is applied. The random zero-field distribution arises from superposition of structured spectra associated with individual total angular momenta. In addition, we show that the resonances with respect to magnetic field in the experimentally accessible range of 400 to 2000 G are chaotically distributed, with strong level repulsion that is characteristic of quantum chaos.