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Microwave shielding is an important technique that can suppress the losses that arise from collisions of ultracold polar molecules. It has been instrumental in achieving molecular Bose-Einstein condensation (BEC) for NaCs [Bigagli et al., Nature 631, 289 (2024)]. We demonstrate that microwave shielding is universal, in the sense that the 2-body collision properties of different molecules are very similar when expressed in suitable reduced units of length and energy. This applies to rate coefficients for inelastic scattering and loss, to scattering lengths, and to the properties of 2-molecule bound states. We also explore the small deviations from universality that arise at very large Rabi frequencies. In general, the collision properties are near-universal except when the Rabi frequency exceeds a few percent of the molecular rotational constant. The universality extends to elliptically polarized microwaves and to combinations of multiple fields. Our results indicate that the methods that have been used to achieve BEC for NaCs can be transferred directly to most other polar molecules.

In mergoassociation, two atoms in separate optical traps are combined to form a molecule when the traps are merged. Previous theoretical treatments have considered only the relative motion of the atoms, neglecting coupling to the motion of the center of mass. We develop a theoretical method to include the coupling to center-of-mass motion and consider its consequences for experiments for both weak and strong coupling. We consider the example of RbCs and then extend the treatment to other systems where mergoassociation may be effective, namely RbSr, RbYb and CsYb. We consider the role of the coupling when the traps are anisotropic and the potential use of moveable traps to construct quantum logic gates.

We investigate the prospect of using ultracold alkali diatomic molecules to implement many-body quantum systems with SU($N$) symmetry. Experimentally accessible molecules offer large $N$ for both bosonic and fermionic systems, with both attractive and repulsive interactions. We carry out coupled-channel scattering calculations on pairs of NaK, NaRb and NaCs molecules that are shielded from destructive collisions with static electric fields. We develop new methods to handle the very large basis sets required to include nuclear spins. We show that all the molecules studied have the properties required for SU($N$) symmetry: the collisions are principally elastic, and the scattering lengths depend only weakly on the spin states of the molecules. The rates of spin-changing inelastic collisions are very low. We develop and test a semiclassical model of the spin dependence and find that it performs well., Comment: 15 pages, 12 figures, and 6 tables

Quantum systems with SU($N$) symmetry are paradigmatic settings for quantum many-body physics. They have been studied for the insights they provide into complex materials and their ability to stabilize exotic ground states. Ultracold alkaline-earth atoms were predicted to exhibit SU($N$) symmetry for $N=2I+1=1,2,\ldots,10$, where $I$ is the nuclear spin. Subsequent experiments have revealed rich many-body physics. However, alkaline-earth atoms realize this symmetry only for fermions with repulsive interactions. In this paper, we predict that ultracold molecules shielded from destructive collisions with static electric fields or microwaves exhibit SU($N$) symmetry, which holds because deviations of the s-wave scattering length from the spin-free values are only about 3\% for CaF with static-field shielding and are estimated to be even smaller for bialkali molecules. They open the door to $N$ as large as $32$ for bosons and $36$ for fermions. They offer important features unachievable with atoms, including bosonic systems and attractive interactions., Comment: 11 pages, 8 figures, 2 tables

Efficient sub-Doppler laser cooling and optical trapping of YO molecules offer new opportunities to study collisional dynamics in the quantum regime. Confined in a crossed optical dipole trap, we achieve the highest phase-space density of $2.5 \times 10^{-5}$ for a bulk laser-cooled molecular sample. This sets the stage to study YO--YO collisions in the microkelvin temperature regime, and reveal state-dependent, single-partial-wave two-body collisional loss rates. We determine the partial-wave contributions to loss of specific rotational states (first excited $N=1$ and ground $N=0$) following two strategies. First, we measure the change of the collision rate in a spin mixture of $N=1$ by tuning the kinetic energy with respect to the p- and d-wave centrifugal barriers. Second, we compare loss rates between a spin mixture and a spin-polarized state in $N=0$. Using quantum defect theory with a partially absorbing boundary condition at short range, we show that the dependence on temperature for $N=1$ can be reproduced in the presence of a d-wave or f-wave resonance, and the dependence on a spin mixture for $N=0$ with a p-wave resonance., Comment: 5 Pages, 4 Figures. Fixed typos. Collisional loss data in $N = 1$ and $N = 0$ is now presented as density versus time instead of number versus time. This work is published in Physical Review A (Copyright 2024 by the American Physical Society). The link to the article is https://journals.aps.org/pra/abstract/10.1103/PhysRevA.110.L041306

Trapped samples of ultracold molecules are often short-lived, because close collisions between them result in trap loss. We investigate the use of shielding with static electric fields to create repulsive barriers between polar molecules to prevent such loss. Shielding is very effective even for RbCs, with a relatively low dipole moment, and even more effective for molecules such as NaK, NaRb and NaCs, with progressively larger dipoles. Varying the electric field allows substantial control over the scattering length, which will be crucial for the stability or collapse of molecular Bose-Einstein condensates. This arises because the dipole-dipole interaction creates a long-range attraction that is tunable with electric field. For RbCs, the scattering length is positive across the range where shielding is effective, because the repulsion responsible for shielding dominates. For NaK, the scattering length can be tuned across zero to negative values. For NaRb and NaCs, the attraction is strong enough to support tetraatomic bound states, and the scattering length passes through resonant poles where these states cross threshold. For KAg and CsAg, there are multiple bound states and multiple poles. For each molecule, we calculate the variation of scattering length with field and comment on the possibilities for exploring new physics., Comment: 12 pages, 8 figures and 1 table

Bose-Einstein condensates of ultracold atoms serve as low-entropy sources for a multitude of quantum-science applications, ranging from quantum simulation and quantum many-body physics to proof-of-principle experiments in quantum metrology and quantum computing. For stability reasons, in the majority of cases the energetically lowest-lying atomic spin state is used. Here we report the Bose-Einstein condensation of caesium atoms in the Zeeman-excited mf = 2 state, realizing a non-ground-state Bose-Einstein condensate with tunable interactions and tunable loss. We identify two regions of magnetic field in which the two-body relaxation rate is low enough that condensation is possible. We characterize the phase transition and quantify the loss processes, finding unusually high three-body losses in one of the two regions. Our results open up new possibilities for the mixing of quantum-degenerate gases, for polaron and impurity physics, and in particular for the study of impurity transport in strongly correlated one-dimensional quantum wires.

Mergoassociation of two ultracold atoms to form a weakly bound molecule can occur when two optical traps that each contain a single atom are merged. Molecule formation occurs at an avoided crossing between a molecular state and the lowest motional state of the atom pair. We develop the theory of mergoassociation for pairs of nonidentical nonspherical traps. We develop a coupled-channel approach for the relative motion of the two atoms and present results for pairs of cylindrically symmetrical traps as a function of their anisotropy. We focus on the strength of the avoided crossing responsible for mergoassociation. We also develop an approximate method that gives insight into the dependence of the crossing strength on aspect ratio.

We study collisions of ultracold CaF molecules in strong static electric fields. These fields allow the creation of long-range barriers in the interaction potential, effectively preventing the molecules from reaching the short-range region where inelastic and other loss processes are likely to occur. We carry out coupled-channel calculations of rate coefficients for elastic scattering and loss. We develop an efficient procedure for including energetically well-separated rotor functions in the basis set via a Van Vleck transformation. We show that shielding is particularly efficient for CaF and allows the rate of two-body loss processes to be reduced by a factor of $10^7$ or more at a field of 23 kV/cm. The loss rates remain low over a substantial range of fields. Electron and nuclear spins cause strong additional loss in some small ranges of field, but have little effect elsewhere. These results pave the way for evaporative cooling of CaF towards quantum degeneracy., Comment: 18 pages, 21 figures

We identify a route for the production of $^{87}$Rb$^{133}$Cs molecules in the $\textrm{X} \, ^1\Sigma^+$ rovibronic ground state that is compatible with efficient mixing of the atoms in optical lattices. We first construct a model for the excited-state structure using constants found by fitting to spectroscopy of the relevant $\textrm{a} \, ^3\Sigma^+ \rightarrow \textrm{b} \, ^3\Pi_1$ transitions at 181.5 G and 217.1 G. We then compare the predicted transition dipole matrix elements from this model to those found for the transitions that have been successfully used for STIRAP at 181.5 G. We form molecules by magnetoassociation on a broad interspecies Feshbach resonance at 352.7 G and explore the pattern of Feshbach states near 305 G. This allows us to navigate to a suitable initial state for STIRAP by jumping across an avoided crossing with radiofrequency radiation. We identify suitable transitions for STIRAP at 305 G. We characterize these transitions experimentally and demonstrate STIRAP to a single hyperfine level of the ground state with a one-way efficiency of 85(4)%., Comment: 21 pages, 8 figures

We consider the magnetically tunable Feshbach resonances that may exist in ultracold mixtures of molecules in $^2\Sigma$ states and alkali-metal atoms. We focus on Rb+CaF as a prototype system. There are likely to be Feshbach resonances analogous to those between pairs of alkali-metal atoms. We investigate the patterns of near-threshold states and the resonances that they cause, using coupled-channel calculations of the bound states and low-energy scattering on model interaction potentials. We explore the dependence of the properties on as-yet-unknown potential parameters. There is a high probability that resonances will exist at magnetic fields below 1000 G, and that these will be broad enough to control collisions and form triatomic molecules by magnetoassociation. We consider the effect of CaF rotation and potential anisotropy, and conclude that they may produce additional resonances but should not affect the existence of rotation-free resonances.

We demonstrate the formation of a single RbCs molecule during the merging of two optical tweezers, one containing a single Rb atom and the other a single Cs atom. Both atoms are initially predominantly in the motional ground states of their respective tweezers. We confirm molecule formation and establish the state of the molecule formed by measuring its binding energy. We find that the probability of molecule formation can be controlled by tuning the confinement of the traps during the merging process, in good agreement with coupled-channel calculations. We show that the conversion efficiency from atoms to molecules using this technique is comparable to magnetoassociation., Comment: 14 pages, 10 figures

We consider the long-range states expected for complexes formed from an alkali-metal diatomic molecule in a singlet state and an alkali-metal atom. We explore the structure of the Hamiltonian for such systems, and the couplings between the six angular momenta that are present. We consider the patterns and densities of the long-range states, and the terms in the Hamiltonian that can cause Feshbach resonances when the states cross threshold as a function of magnetic field. We present a case study of $^{40}$K$^{87}$Rb+$^{87}$Rb. We show multiple types of resonance due to long-range states with rotational and/or hyperfine excitation, and consider the likelihood of them existing at low to moderate magnetic fields.

Magnetically tunable Feshbach resonances exist in ultracold collisions between atoms in $^2$S and $^3$P$_0$ states, such as an alkali-metal atom colliding with Yb or Sr in a clock state. We investigate the mechanisms of these resonances and identify the terms in the collision Hamiltonian responsible for them. They involve indirect coupling between the open and closed channels, via intermediate channels involving atoms in $^3$P$_1$ states. The resonance widths are generally proportional to the square of the magnetic field and are strongly enhanced when the magnitude of the background scattering length is large. For any given pair of atoms, the scattering length can be tuned discretely by choosing different isotopes of the $^3$P$_0$ atom. For each combination of an alkali-metal atom and either Yb or Sr, we consider the prospects of finding an isotopic combination that has both a large background scattering length and resonances at high but experimentally accessible field. We conclude that $^{87}$Rb+Yb, Cs+Yb and $^{85}$Rb+Sr are particularly promising combinations., Comment: 11 pages, 9 figures and 2 tables

Using a combination of bound-state spectroscopy and loss spectroscopy, we pinpoint eight intrastate Feshbach resonances in $^{39}$K, as well as six previously unexplored interstate ones. We also perform a detailed characterization of four of the intrastate resonances and two of the interstate ones. We carry out coupled-channel scattering calculations and find good agreement with experiment. The combination of experiment and theory provides a faithful map of the scattering length $a$ and permits precision measurements of the signatures of Efimov physics across four intermediate-strength resonances. We measure the modulation of the $a^4$ scaling of the three-body loss coefficient for both $a<0$ and $a>0$, as well as the many-body loss dynamics at unitarity (where $a$ diverges). The absolute positions of the observed Efimov features confirm a ubiquitous breakdown of Efimov--van-der-Waals universality in $^{39}$K, while their relative positions are in agreement with the universal Efimov ratios. The loss dynamics at the three broadest Feshbach resonances are universal within experimental uncertainties, consistent with observing little variation in the Efimov width parameters., Comment: 12 pages, 7 figures (including appendices)

We report the first observation of magnetic Feshbach resonances between ${}^{173}$Yb and $^{133}$Cs. In a mixture of Cs atoms prepared in the $(f=3, m_f=3)$ state and unpolarized fermionic ${}^{173}$Yb we observe resonant atom loss due to two sets of magnetic Feshbach resonances around 622~G and 702~G. Resonances for individual Yb nuclear spin components $m_{i,\mathrm{Yb}}$ are split by its interaction with the Cs electronic spin, which also provides the main coupling mechanism for the observed resonances. The observed splittings and relative resonance strengths are in good agreement with theoretical predictions from coupled-channel calculations., Comment: 7 pages, 2 figures

We present a computer program to calculate the quantised rotational and hyperfine energy levels of $^{1}\Sigma $ diatomic molecules in the presence of dc electric, dc magnetic, and off-resonant optical fields. Our program is applicable to the bialkali molecules used in ongoing state-of-the-art experiments with ultracold molecular gases. We include functions for the calculation of space-fixed electric dipole moments, magnetic moments and transition dipole moments.

We prepare pairs of $^{133}$Cs atoms in a single optical tweezer and perform Feshbach spectroscopy for collisions of atoms in the states $(f=3, m_f=\pm3)$. We detect enhancements in pair loss using a detection scheme where the optical tweezers are repeatedly subdivided. For atoms in the state $(3,-3)$, we identify resonant features by performing inelastic loss spectroscopy. We carry out coupled-channel scattering calculations and show that at typical experimental temperatures the loss features are mostly centred on zeroes in the scattering length, rather than resonance centres. We measure the number of atoms remaining after a collision, elucidating how the different loss processes are influenced by the tweezer depth. These measurements probe the energy released during an inelastic collision, and thus give information on the states of the collision products. We also identify resonances with atom pairs prepared in the absolute ground state $(f=3, m_f=3)$, where two-body radiative loss is engineered by an excitation laser blue-detuned from the Cs D$_2$ line. These results demonstrate optical tweezers to be a versatile tool to study two-body collisions with number-resolved detection sensitivity., Comment: 18 pages, 6 figures

We obtain the interaction potential for NaCs by fitting to experiments on ultracold scattering and spectroscopy in optical tweezers. The central region of the potential has been accurately determined from Fourier-Transform spectroscopy at higher temperatures, so we focus on adjusting the long-range and short-range parts. We use coupled-channel calculations of binding energies and wave functions to understand the nature of the molecular states observed in ultracold spectroscopy, and of the state that causes the Feshbach resonance used to create ultracold NaCs molecules. We elucidate the relationships between the experimental quantities and features of the interaction potential. We establish the combinations of experimental quantities that determine particular features of the potential. We find that the long-range dispersion coefficient $C_6$ must be increased by about 0.9% to 3256(1) $E_\textrm{h} a_0^6$ to fit the experimental results. We use coupled-channel calculations on the final potential to predict bound-state energies and resonance positions.

We have investigated magnetically tunable Feshbach resonances in ultracold collisions of Rb with Yb in its metastable $^3$P$_2$ and $^3$P$_0$ states, using coupled-channel scattering and bound-state calculations. For the $^3$P$_2$ state, we find sharp resonances when both atoms are in their lowest Zeeman sublevels. However, these resonances are decayed by inelastic processes that produce Yb atoms in $^3$P$_1$ and $^3$P$_0$ states. The molecules that might be produced by magnetoassociation at the $^3$P$_2$ thresholds can decay by similar pathways and would have lifetimes no more than a few microseconds. For the $^3$P$_0$ state, by contrast, there are resonances that are promising for magnetoassociation. There are resonances due to both rotating and non-rotating molecular states that are significantly stronger than the analogous resonances for Yb($^1$S). The ones due to rotating states are denser in magnetic field; in contrast to Yb($^1$S), they exist even for bosonic isotopes of Yb($^3$P$_0$)., Comment: 15 pages and 8 figures

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 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 values 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., Comment: Accepted manuscript

The ultracold mixture of \Na and \Rb atoms has become an important system for investigating physics in Bose-Bose atomic mixtures and for forming ultracold ground-state polar molecules. In this work, we provide an improved characterization of the most commonly used Feshbach resonance near 347.64 G between \Na and \Rb in their absolute ground states. We form Feshbach molecules using this resonance and measure their binding energies by dissociating them via magnetic field modulation. We use the binding energies to refine the singlet and triplet potential energy curves, using coupled-channel bound-state calculations. We then use coupled-channel scattering calculations on the resulting potentials to produce a high-precision mapping between magnetic field and scattering length. We also observe 10 additional $s$-wave Feshbach resonances for \Na and \Rb in different combinations of Zeeman sublevels of the $F = 1$ hyperfine states. Some of the resonances show 2-body inelastic decay due to spin exchange. We compare the resonance properties with coupled-channel scattering calculations that full take account of inelastic properties., Comment: 10 pages, 6 figures

The beyond-mean-field Lee-Huang-Yang (LHY) correction is ubiquitous in dilute ultracold quantum gases. However, its effects are often elusive due to the typically much larger influence of the mean-field energy. In this work, we study an ultracold mixture of $^{23}$Na and $^{87}$Rb with tunable attractive interspecies interactions. The LHY effects manifest in the formation of self-bound quantum liquid droplets and the expansion dynamics of the gas-phase sample. A liquid-to-gas phase diagram is obtained by measuring the critical atom numbers below which the self-bound behavior disappears. In stark contrast to trapped gas-phase condensates, the gas-phase mixture formed following the liquid-to-gas phase transition shows an anomalous expansion featuring a larger release energy for increasing mean-field attractions., Comment: 8 pages, 7 figures

We study inelastic collisions between CaF molecules and $^{87}$Rb atoms in a dual-species magneto-optical trap. The presence of atoms increases the loss rate of molecules from the trap. By measuring the loss rates and density distributions, we determine a collisional loss rate coefficient $k_{2} = (1.43 \pm 0.29) \times 10^{-10}$ cm$^{3}$/s at a temperature of 2.4 mK. We show that this is not substantially changed by light-induced collisions or by varying the populations of excited-state atoms and molecules. The observed loss rate is close to the universal rate expected in the presence of fast loss at short range, and can be explained by rotation-changing collisions in the ground electronic state., Comment: 14 pages, 6 figures. Added a new figure and some further details about the methods; expanded our discussion of the results

We report the preparation of exactly one $^{87}$Rb atom and one $^{133}$Cs atom in the same optical tweezer as the essential first step towards the construction of a tweezer array of individually trapped $^{87}$Rb$^{133}$Cs molecules. Through careful selection of the tweezer wavelengths, we show how to engineer species-selective trapping potentials suitable for high-fidelity preparation of Rb $+$ Cs atom pairs. Using a wavelength of 814~nm to trap Rb and 938~nm to trap Cs, we achieve loading probabilities of $0.508(6)$ for Rb and $0.547(6)$ for Cs using standard red-detuned molasses cooling. Loading the traps sequentially yields exactly one Rb and one Cs atom in $28.4(6)\,\%$ of experimental runs. Using a combination of an acousto-optic deflector and a piezo-controlled mirror to control the relative position of the tweezers, we merge the two tweezers, retaining the atom pair with a probability of $0.99^{(+0.01)}_{(-0.02)}$. We use this capability to study hyperfine-state-dependent collisions of Rb and Cs in the combined tweezer and compare the measured two-body loss rates with coupled-channel quantum scattering calculations., Comment: 22 pages, 6 figures

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 triatomic 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., Comment: 10 pages, 3 figures

Quantum states with long-lived coherence are essential for quantum computation, simulation and metrology. The nuclear spin states of ultracold molecules prepared in the singlet rovibrational ground state are an excellent candidate for encoding and storing quantum information. However, it is important to understand all sources of decoherence for these qubits, and then eliminate them, in order to reach the longest possible coherence times. Here, we fully characterise the dominant mechanisms for decoherence of a storage qubit in an optically trapped ultracold gas of RbCs molecules using high-resolution Ramsey spectroscopy. Guided by a detailed understanding of the hyperfine structure of the molecule, we tune the magnetic field to where a pair of hyperfine states have the same magnetic moment. These states form a qubit, which is insensitive to variations in magnetic field. Our experiments reveal an unexpected differential tensor light shift between the states, caused by weak mixing of rotational states. We demonstrate how this light shift can be eliminated by setting the angle between the linearly polarised trap light and the applied magnetic field to a magic angle of $\arccos{(1/\sqrt{3})}\approx55^{\circ}$. This leads to a coherence time exceeding 6.9 s (90% confidence level). Our results unlock the potential of ultracold molecules as a platform for quantum computation., Comment: 19 pages, 12 figures

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~$\mu$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., Comment: 9 pages, 6 figures. Minor changes following review

We report coherent association of atoms into a single weakly bound NaCs molecule in an optical tweezer through an optical Raman transition. The Raman technique uses a deeply bound electronic excited intermediate state to achieve a large transition dipole moment while reducing photon scattering. Starting from two atoms in their relative motional ground state, we achieve an optical transfer efficiency of 69%. The molecules have a binding energy of 770.2MHz at 8.83(2)G. This technique does not rely on Feshbach resonances or narrow excited-state lines and may allow a wide range of molecular species to be assembled atom-by-atom.

We study three-atom inelastic scattering in ultracold \textsuperscript{39}K near a Feshbach resonance of intermediate coupling strength. The non-universal 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 \textsuperscript{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., Comment: 14 pages, 9 figures, 3 tables

We investigate the effects of static electric and magnetic fields on the differential ac Stark shifts for microwave transitions in ultracold bosonic $^{87}$Rb$^{133}$Cs molecules, for light of wavelength $\lambda = 1064~\mathrm{nm}$. Near this wavelength we observe unexpected two-photon transitions that may cause trap loss. We measure the ac Stark effect in external magnetic and electric fields, using microwave spectroscopy of the first rotational transition. We quantify the isotropic and anisotropic parts of the molecular polarizability at this wavelength. We demonstrate that a modest electric field can decouple the nuclear spins from the rotational angular momentum, greatly simplifying the ac Stark effect. We use this simplification to control the ac Stark shift using the polarization angle of the trapping laser.

We demonstrate the formation of a single NaCs molecule in an optical tweezer by magnetoassociation through an s-wave Feshbach resonance at 864.11(5)G. Starting from single atoms cooled to their motional ground states, we achieve conversion efficiencies of 47(1)%, and measure a molecular lifetime of 4.7(7)ms. By construction, the single molecules are predominantly (77(5)%) in the center-of-mass motional ground state of the tweezer. Furthermore, we produce a single p-wave molecule near 807G by first preparing one of the atoms with one quantum of motional excitation. Our creation of a single weakly bound molecule in a designated internal state in the motional ground state of an optical tweezer is a crucial step towards coherent control of single molecules in optical tweezer arrays.

We report the observation of microwave coherent control of rotational states of ultracold $^{85}$Rb$^{133}$Cs molecules formed in their vibronic ground state by short-range photoassociation. Molecules are formed in the single rotational state $X(v=0,J=1)$ by exciting pairs of atoms to the short-range state $(2)^{3}\Pi_{0^{-}} (v=11, J=0)$, followed by spontaneous decay. We use depletion spectroscopy to record the dynamic evolution of the population distribution and observe clear Rabi oscillations while irradiating on a microwave transition between coupled neighbouring rotational levels. A density-matrix formalism that accounts for longitudinal and transverse decay times reproduces both the dynamic evolution during the coherent process and the equilibrium population. The coherent control reported here is valuable both for investigating coherent quantum effects and for applications of cold polar molecules produced by continuous short-range photoassociation., Comment: 5 pages, 4 figures

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., Comment: 13 pages, 5 figures

Radiofrequency (RF)-dressed potentials are a promising technique for manipulating atomic mixtures, but so far little work has been undertaken to understand the collisions of atoms held within these traps. In this work, we dress a mixture of 85Rb and 87Rb with RF radiation, characterize the inelastic loss that occurs, and demonstrate species-selective manipulations. Our measurements show the loss is caused by two-body 87Rb+85Rb collisions, and we show the inelastic rate coefficient varies with detuning from the RF resonance. We explain our observations using quantum scattering calculations, which give reasonable agreement with the measurements. The calculations consider magnetic fields both perpendicular to the plane of RF polarization and tilted with respect to it. Our findings have important consequences for future experiments that dress mixtures with RF fields., Comment: 12 pages, 7 figures, 1 table

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.

We report our experimental results on the collisional physics between non-S-state atoms (ytterbium (Yb), effectively a two-electron system, in the metastable ${}^3\mathrm{P}_2$ state) and S-state atoms (lithium (Li), an alkali metal, in the ground state). At low magnetic fields, by measuring inelastic interspecies collisional losses in the double quantum degenerate mixture we reveal the strong dependence of the inelastic losses on the internal spin states of both species and suppressed losses in stretched state configurations. Increasing the magnetic field up to 800 G we further investigate the magnetic field dependence of the collisional interactions. There, smoothly increasing inelastic losses are observed towards higher fields. The combined knowledge of both the magnetic field and the spin state dependence of the collisional losses of this prototypical mixture system of non-S-state and S-state atoms provides a significant step forward towards controllable impurity physics realized in the Yb-Li ultracold system., Comment: 9 pages, 5 figures

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 discuss how the internal structure of ultracold molecules, trapped in the motional ground state of optical tweezers, can be used to implement qudits. We explore the rotational, fine and hyperfine structure of $^{40}$Ca$^{19}$F and $^{87}$Rb$^{133}$Cs, which are examples of molecules with $^2\Sigma$ and $^1\Sigma$ electronic ground states, respectively. In each case we identify a subset of levels within a single rotational manifold suitable to implement a 4-level qudit. Quantum gates can be implemented using two-photon microwave transitions via levels in a neighboring rotational manifold. We discuss limitations to the usefulness of molecular qudits, arising from off-resonant excitation and decoherence. As an example, we present a protocol for using a molecular qudit of dimension $d=4$ to perform the Deutsch algorithm.

Polar molecules in superpositions of rotational states exhibit long-range dipolar interactions, but maintaining their coherence in a trapped sample is a challenge. We present calculations that show many laser-coolable molecules have convenient rotational transitions that are exceptionally insensitive to magnetic fields. We verify this experimentally for CaF where we find a transition with sensitivity below 5 Hz G$^{-1}$ and use it to demonstrate a rotational coherence time of 6.4(8) ms in a magnetic trap. Simulations suggest it is feasible to extend this to more than 1 s using a smaller cloud in a biased magnetic trap.

We investigate the use of microwave radiation to produce a repulsive shield between pairs of ultracold polar molecules and prevent collisional losses that occur when molecular pairs reach short range. We carry out coupled-channels calculations on RbCs+RbCs and CaF+CaF collisions in microwave fields. We show that effective shielding requires predominantly circular polarization, but can still be achieved with elliptical polarization that is around 90% circular.

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 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 Cs+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 2-body inelastic loss, while the real part allows us to identify regions of magnetic field where 3-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 $(3,-3)$ states where high-density clouds should be long-lived., Comment: 7 pages, 3 figures

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., Comment: 15 pages, 7 figures, 1 table

MOLSCAT is a general-purpose package for performing non-reactive quantum scattering calculations for atomic and molecular collisions using coupled-channel methods. Simple atom-molecule and molecule-molecule collision types are coded internally and additional ones may be handled with plug-in routines. Plug-in routines may include external magnetic, electric or photon fields (and combinations of them). Simple interaction potentials are coded internally and more complicated ones may be handled with plug-in routines. BOUND is a general-purpose package for performing calculations of bound-state energies in weakly bound atomic and molecular systems using coupled-channel methods. It solves the same sets of coupled equations as MOLSCAT, and can use the same plug-in routines if desired, but with different boundary conditions. FIELD is a development of BOUND that locates external fields at which a bound state exists with a specified energy. One important use is to locate the positions of magnetically tunable Feshbach resonance positions in ultracold collisions. Versions of these programs before version 2019.0 were released separately. However, there is a significant degree of overlap between their internal structures and usage specifications. This manual therefore describes all three, with careful identification of parts that are specific to one or two of the programs., Comment: 209 pages. Program source code available from https://github.com/molscat/molscat This is the full program documentation for the programs described in the journal papers Comp. Phys. Commun. 241, 1-8 (2019) (arXiv:1811.09111) and Comp. Phys. Commun. 241, 9-16 (2019) (arXiv:1811.09584). There is significant text overlap between some parts of the documentation and the (much shorter) journal papers

MOLSCAT is a general-purpose program for quantum-mechanical calculations on nonreactive atom-atom, atom-molecule and molecule-molecule collisions. It constructs the coupled-channel equations of atomic and molecular scattering theory, and solves them by propagating the wavefunction or log-derivative matrix outwards from short range to the asymptotic region. It then applies scattering boundary conditions to extract the scattering matrix (S matrix). Built-in coupling cases include atom + rigid linear molecule, atom + vibrating diatom, atom + rigid symmetric top, atom + asymmetric or spherical top, rigid diatom + rigid diatom, rigid diatom + asymmetric top, and diffractive scattering of an atom from a crystal surface. Interaction potentials may be specified either in program input (for simple cases) or with user-supplied routines. For the built-in coupling cases, MOLSCAT can loop over partial wave (or total angular momentum) to calculate elastic and inelastic cross integral sections and spectroscopic line-shape cross sections. Post-processors are available to calculate differential cross sections, transport, relaxation and Senftleben-Beenakker cross sections, and to fit the parameters of scattering resonances. MOLSCAT also provides an interface for plug-in routines to specify coupling cases (Hamiltonians and basis sets) that are not built in; plug-in routines are supplied to handle collisions of a pair of alkali-metal atoms with hyperfine structure in an applied magnetic field. For low-energy scattering, MOLSCAT can calculate scattering lengths and effective ranges and can locate and characterize scattering resonances as a function of an external variable such as the magnetic field., Comment: arXiv admin note: substantial text overlap with arXiv:1811.09111 This is because these are two parallel papers that describe related programs with the same theoretical basis but for different purposes

The BOUND program calculates the bound states of a complex formed from two interacting particles using coupled-channel methods. It is particularly suitable for the bound states of atom-molecule and molecule-molecule Van der Waals complexes and for the near-threshold bound states that are important in ultracold physics. It uses a basis set for all degrees of freedom except $R$, the separation of the centres of mass of the two particles. The Schr\"odinger equation is expressed as a set of coupled equations in $R$. Solutions of the coupled equations are propagated outwards from the classically forbidden region at short range and inwards from the classically forbidden region at long range, and matched at a point in the central region. Built-in coupling cases include atom + rigid linear molecule, atom + vibrating diatom, atom + rigid symmetric top, atom + asymmetric or spherical top, rigid diatom + rigid diatom, and rigid diatom + asymmetric top. Both programs provide an interface for plug-in routines to specify coupling cases (Hamiltonians and basis sets) that are not built in. With appropriate plug-in routines, BOUND can take account of the effects of external electric, magnetic and electromagnetic fields, locating bound-state energies at fixed values of the fields. The related program FIELD uses the same plug-in routines and locates values of the fields where bound states exist at a specified energy. As a special case, it can locate values of the external field where bound states cross scattering thresholds and produce zero-energy Feshbach resonances. Plug-in routines are supplied to handle the bound states of a pair of alkali-metal atoms with hyperfine structure in an applied magnetic field., Comment: One of two parallel papers that document the MOLSCAT, BOUND and FIELD programs, which use closely related theoretical methods but serve different purposes. This paper and arXiv:1811.09584 therefore have substantial text overlap