We explore the character of a novel set of ``field-linked'' states that were predicted in [A. V. Avdeenkov and J. L. Bohn, Phys. Rev. Lett. 90, 043006 (2003)]. These states exist at ultralow temperatures in the presence of an electrostatic field, and their properties are strongly dependent on the field's strength. We clarify the nature of these quasi-bound states by constructing their wave functions and determining their approximate quantum numbers. As the properties of field-linked states are strongly defined by anisotropic dipolar and Stark interactions, we construct adiabatic surfaces as functions of both the intermolecular distance and the angle that the intermolecular axis makes with the electric field. Within an adiabatic approximation we solve the 2-D Schrodinger equation to find bound states, whose energies correlate well with resonance features found in fully-converged multichannel scattering calculations.
We describe the realization of a dc electric-field trap for ultracold polar molecules, the thin-wire electrostatic trap (TWIST). The thin wires that form the electrodes of the TWIST allow us to superimpose the trap onto a magneto-optical trap (MOT). In our experiment, ultracold polar NaCs molecules in their electronic ground state are created in the MOT via photoassociation, achieving a continuous accumulation in the TWIST of molecules in low-field seeking states. Initial measurements show that the TWIST trap lifetime is limited only by the background pressure in the chamber.
We have produced ultracold, polar RbCs* molecules via photoassociation in a laser-cooled mixture of Rb and Cs atoms. Using a model of the RbCs* molecular interaction which reproduces the observed rovibrational structure, we infer decay rates in our experiments into deeply bound singlet ground state RbCs vibrational levels as high as 5 x 10^5 s^-1 per level. Population in such deeply bound levels could be efficiently transferred to the vibrational ground state using a single stimulated Raman transition, opening the possibility to create large samples of stable, ultracold polar molecules.
We determine trapping conditions for ultracold polar molecules, where pairs of internal states experience identical trapping potentials. Such conditions could ensure that detrimental effects of inevitable inhomogeneities across an ultracold sample are significantly reduced. In particular, we investigate the internal rovibronic and hyperfine quantum states of ultracold fermionic ground-state $^{40}$K$^{87}$Rb polar molecules, when static magnetic, static electric, and trapping laser fields are simultaneously applied. Understanding the effect of changing the relative orientation or polarization …
We present a detailed description on how to build a Thin WIre electroStatic Trap (TWIST) for ultracold polar molecules. It is the first design of an electrostatic trap that can be superimposed directly onto a magneto optical trap (MOT). We can thus continuously produce ultracold polar molecules via photoassociation from a two species MOT and instantaneously trap them in the TWIST without the need for complex transfer schemes. Despite the spatial overlap of the TWIST and the MOT, the two traps can be operated and optimized completely independently due to the complementary nature of the utilized…
Scattering resonances are an essential tool for controlling interactions of ultracold atoms and molecules. However, conventional Feshbach scattering resonances, which have been extensively studied in various platforms, are not expected to exist in most ultracold polar molecules due to the fast loss that occurs when two molecules approach at a close distance. Here, we demonstrate a new type of scattering resonances that is universal for a wide range of polar molecules. The so-called field-linked resonances occur in the scattering of microwave-dressed molecules due to stable macroscopic tetramer…
We discuss consequences of Fermi exchange symmetry on collisions of polar molecules at low temperatures (below 1 K), considering the OD radical as a prototype. At low fields and low temperatures, Fermi statistics can stabilize a gas of OD molecules against state-changing collisions. We find, however, that this stability does not extend to temperatures high enough to assist with evaporative cooling. In addition, we establish that a novel ``field-linked'' resonance state of OD dimers exists, in analogy with the similar states predicted for bosonic OH.
The collisions between linear polar molecules, trapped in a microwave field with circular polarization, are theoretically analyzed. The microwave trap suggested by DeMille \cite{DeMille} seems to be rather advantageous in comparison with other traps. Here we have demonstrated that the microwave trap can provide a successful evaporative cooling for polar molecules in a rather broad range of frequencies of the AC-field. We suggested that not only ground state polar molecules but also molecules in some other states can be safely trapped. But the state in which molecules can be safely loaded and t…
We have demonstrated microwave-assisted coherent control of ultracold $^{85}$Rb$^{133}$Cs molecules with a ladder-type configuration of rotational states. A probe microwave (MW) field is used to couple a lower state $X^1Σ^+(v=0, J=1)$ and a middle state $X^1Σ^+(v=0, J=2)$, while a control MW field couples the middle state and a upper state $X^1Σ^+(v=0, J=3)$. In the presence of the control field, the population of middle rotational states, $X^1Σ^+(v=0, J=2)$, can be reduced by a control MW field. Broadening of spectral splitting and shift of central frequency in this coherent spectrum are obse…
The prospects of sympathetic cooling of polar molecules with magnetically co-trapped alkali-metal atoms are generally considered poor due to strongly anisotropic atom-molecule interactions leading to large spin relaxation rates. Using rigorous quantum scattering calculations based on ab initio interaction potentials, we show that inelastic spin relaxation in low-temperature collisions of CaH(2Sigma) molecules with Li and Mg atoms occurs at a slow rate despite the strongly anisotropic interactions. This unexpected result, which we rationalize using multichannel quantum defect theory, opens up t…
The properties of the electronic ground state of the polar and paramagnetic chromium--closed-shell-atom molecules have been investigated. State-of-the-art \textit{ab initio} techniques have been applied to compute the potential energy curves for the chromium--alkaline-earth-metal-atom, CrX (X = Be, Mg, Ca, Sr, Ba), and chromium--ytterbium, CrYb, molecules in the Born-Oppenheimer approximation for the $X^7Σ^+$ high-spin electronic ground state. The spin restricted open-shell coupled cluster method restricted to single, double, and noniterative triple excitations, RCCSD(T), was employed and the …
We have successfully implemented the first simultaneous magneto-optical trapping (MOT) of lithium ($^6$Li) and ytterbium ($^{174}$Yb) atoms, towards production of ultracold polar molecules of LiYb. For this purpose, we developed the dual atomic oven which contains both atomic species as an atom source and successfully observed the spectra of the Li and Yb atoms in the atomic beams from the dual atomic oven. We constructed the vacuum chamber including the glass cell with the windows made of zinc selenium (ZnSe) for the CO$_2$ lasers, which are the useful light sources of optical trapping for ev…
The collisional stability of ultracold polar molecules in electrostatic traps is considered. Rate constants for collisions that drive molecules from weak-field-seeking to strong-field-seeking states are estimated using a simple model. The rates are found to be quite large, of order 10^{-12} - 10^{-10} cm^3/sec, and moreover to grow rapidly in an externally applied electric field. It is argued that these results are generic for polar molecules, and that therefore polar molecules should be trapped by other than electrostatic means.
We consider ultracold collisions of ground-state, heteronuclear alkali dimers that are susceptible to four-center chemical reactions 2 AB -> A2 + B2 even at sub-microKelvin temperature. These reactions depend strongly on species, temperature, electric field, and confinement in an optical lattice. We calculate ab initio van der Walls coefficients for these interactions, and use a quantum formalism to study the scattering properties of such molecules under an external electric field and optical lattice. We also apply a quantum threshold model to explore the dependence of reaction rates on the va…
We predict that pairs of polar molecules can be weakly bound together in an ultracold environment, provided that a dc electric field is present. The field that links the molecules together also strongly influences the basic properties of the resulting dimer, such as its binding energy and predissociation lifetime. Because of their long-range character these dimers will be useful in disentangling cold collision dynamics of polar molecules. As an example, we estimate the microwave photoassociation yield for OH-OH cold collisions.
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 demonstrate the production of ultracold polar RbCs molecules in their vibronic ground state, via photoassociation of laser-cooled atoms followed by a laser-stimulated state transfer process. The resulting sample of $X ^1Σ^+ (v=0)$ molecules has a translational temperature of $\sim100 μ$K and a narrow distribution of rotational states. With the method described here it should be possible to produce samples even colder in all degrees of freedom, as well as other bi-alkali species.
We report measurements of the ac polarizabilities of ultracold ground-state $^{23}\rm{Na}^{87}\rm{Rb}$ molecules. While the polarizability of the ground rotational state $J = 0$ is isotropic, that of the first excited rotational state $J = 1$ is anisotropic and depends strongly on the light polarization angle. We obtain both polarizabilities precisely by combining trap oscillation frequency measurement and high resolution rotational spectroscopy driven by microwave. With the optimized light polarization angle and intensity combination, the nonuniformity of the differential ac Stark shift betwe…
We investigate the rovibrational population redistribution of polar molecules in the electronic ground state induced by spontaneous emission and blackbody radiation. As a model system we use optically trapped LiCs molecules formed by photoassociation in an ultracold two-species gas. The population dynamics of vibrational and rotational states is modeled using an ab-initio electric dipole moment function and experimental potential energy curves. Comparison with the evolution of the v"=3 electronic ground state yields good qualitative agreement. The analysis provides important input to assess ap…
A systematic study of the leading isotropic van der Waals coefficients for the alkali-metal atom + molecule and molecule + molecule systems is presented. Dipole moments and static and dynamic dipole polarizabilities are calculated employing high-level quantum chemistry calculations. The dispersion, induction, and rotational parts of the isotropic van der Waals coefficient are evaluated. The known van der Waals coefficients are then used to derive characteristics essential for simple models of the collisions involving the corresponding ultracold polar molecules.
The rapid development of experimental techniques to produce ultracold alkali molecules opens the ways to manipulate them and to control their dynamics using external electric fields. A prerequisite quantity for such studies is the knowledge of their static dipole polarizabilities. In this paper, we computed the variations with internuclear distance and with vibrational index of the static dipole polarizability components of all homonuclear alkali dimers including Fr$_2$, and of all heteronuclear alkali dimers involving Li to Cs, in their electronic ground state and in their lowest triplet stat…
We predict the existence of a class of ultracold giant molecules formed from trapped ultracold Rydberg atoms and polar molecules. The interaction which leads to the formation of such molecules is the anisotropic charge-dipole interaction ($a/R^2$). We show that prominent candidate molecules such as KRb and deuterated hydroxyl (OD) should bind to Rydberg rubidium atoms, with energies $E_b\simeq 5-25$ GHz at distances $R\simeq 0.1-1 \ μ$m. These molecules form in double wells, mimicking chiral molecules, with each well containing a particular dipole orientation. We prepare a set of correlated dr…
We use microwaves to engineer repulsive long-range interactions between ultracold polar molecules. The resulting shielding suppresses various loss mechanisms and provides large elastic cross sections. Hyperfine interactions limit the shielding under realistic conditions, but a magnetic field allows suppression of the losses to below 10-14 cm3 s-1. The mechanism and optimum conditions for shielding differ substantially from those proposed by Gorshkov et al. [Phys. Rev. Lett. 101, 073201 (2008)], and do not require cancelation of the long-range dipole-dipole interaction that is vital to many app…
We investigate the effect of far-off-resonant trapping light on ultracold bosonic RbCs molecules. We use kHz-precision microwave spectroscopy to measure the differential AC Stark shifts between the ground and first excited rotational levels of the molecule with hyperfine-state resolution. We demonstrate through both experiment and theory that coupling between neighboring hyperfine states manifests in rich structure with many avoided crossings. This coupling may be tuned by rotating the polarization of the linearly polarized trapping light. A combination of spectroscopic and parametric heating …
We consider ultracold collisions of polar molecules confined in a one dimensional optical lattice. Using a quantum scattering formalism and a frame transformation method, we calculate elastic and chemical quenching rate constants for fermionic molecules. Taking KRb molecules as a prototype, we find that the rate of quenching collisions is enhanced at zero electric field as the confinement is increased, but that this rate is suppressed when the electric field is turned on. For molecules with 500 nK of collision energy, for realistic molecular densities, and for achievable experimental electric …
We show theoretically that ultracold hydrogen atoms have very favorable properties for sympathetic cooling of molecules to microkelvin temperatures. We calculate the potential energy surfaces for spin-polarized interactions of H atoms with the prototype molecules NH(triplet-Sigma-) and OH(doublet-Pi) and show that they are shallow (50 to 80 cm-1) and only weakly anisotropic. We carry out quantum collision calculations on H+NH and H+OH and show that the ratio of elastic to inelastic cross sections is high enough to allow sympathetic cooling from temperatures well over 1 K for NH and around 250 …
We present an architecture for the quantum simulation of many-body spin interactions based on ultracold polar molecules trapped in optical lattices. Our approach employs digital quantum simulation, i.e., the dynamics of the simulated system is reproduced by the quantum simulator in a stroboscopic pattern, and allows to simulate both coherent and dissipative dynamics. We discuss the realization of Kitaev's toric code Hamiltonian, a paradigmatic model involving four-body interactions, and we analyze the requirements for an experimental implementation.
Analytic expressions describe universal elastic and reactive rates of quasi-two-dimensional and quasi-one-dimensional collisions of highly reactive ultracold molecules interacting by a van der Waals potential. Exact and approximate calculations for the example species of KRb show that stability and evaporative cooling can be realized for spin-polarized fermions at moderate dipole and trapping strength, whereas bosons or unlike fermions require significantly higher dipole or trapping strengths.
Ultracold polar molecules (UPMs) are emerging as a novel and powerful platform for fundamental applications in quantum science. Here, we report characterization of the coherence between nuclear spin levels of ultracold ground-state sodium-rubidium molecules loaded into a 3D optical lattice with a nearly photon scattering limited trapping lifetime of 9(1) seconds. After identifying and compensating the main sources of decoherence, we achieve a maximum nuclear spin coherence time of $T_2^* = 3.3(6)$~s with two-photon Ramsey spectroscopy. Furthermore, based on the understanding of the main factor…
We consider collisions of electric and magnetic polar molecules, taking the OH radical as an example, subject to combined electric and magnetic static fields. We show that the relative orientation of the fields has an important effect on the collision processes for different fields magnitude at different collision energies. This is due to the way the molecules polarize in the combined electric and magnetic fields and hence the way the electric dipole-dipole interaction rises. If OH molecules are confined in magnetic quadrupole traps and if an electric field is applied, molecular collisions wil…
Ultracold LiCs molecules in the absolute ground state X$^1Σ^+$, v"=0, J"=0 are formed via a single photo-association step starting from laser-cooled atoms. The selective production of v"=0, J"=2 molecules with a 50-fold higher rate is also demonstrated. The rotational and vibrational state of the ground state molecules is determined in a setup combining depletion spectroscopy with resonant-enhanced multi-photon ionization time-of-flight spectroscopy. Using the determined production rate of up to 5x10^3 molecules/s, we describe a simple scheme which can provide large samples of externally and i…
Selection of "magic" trapping conditions with ultracold atoms or molecules, where pairs of internal states experience identical trapping potentials, brings substantial benefits to precision measurements and quantum computing schemes. Working at such conditions could ensure that detrimental effects of inevitable inhomogeneities across an ultracold sample are significantly reduced. However, this aspect of confinement remains unexplored for ultracold polar molecules. Here, we present means to control the AC Stark shift of rotational states of ultracold polar molecules, when subjected to both trap…
We report the measurement of the anisotropic AC polarizability of ultracold polar $^{40}$K$^{87}$Rb molecules in the ground and first rotationally excited states. Theoretical analysis of the polarizability agrees well with experimental findings. Although the polarizability can vary by more than 30%, a "magic" angle between the laser polarization and the quantization axis is found where the polarizability of the $|N=0,m_N=0>$ and the $|N=1,m_N=0>$ states match. At this angle, rotational decoherence due to the mismatch in trapping potentials is eliminated, and we observe a sharp increase in the …
We demonstrate one-dimensional sub-Doppler laser cooling of a beam of YbF molecules to 100 $μ$K. This is a key step towards a measurement of the electron's electric dipole moment using ultracold molecules. We compare the effectiveness of magnetically-assisted and polarization-gradient sub-Doppler cooling mechanisms. We model the experiment and find good agreement with our data.
Heteronuclear alkali-metal dimers represent the class of molecules of choice for creating samples of ultracold molecules exhibiting an intrinsic large permanent electric dipole moment. Among them, the KCs molecule, with a permanent dipole moment of 1.92~Debye still remains to be observed in ultracold conditions. Based on spectroscopic studies available in the literature completed by accurate quantum chemistry calculations, we propose several optical coherent schemes to create ultracold bosonic and fermionic KCs molecules in their absolute rovibrational ground level, starting from a weakly boun…
This paper reviews recent advances in the study of strongly interacting systems of dipolar molecules. Heteronuclear molecules feature large and tunable electric dipole moments, which give rise to long-range and anisotropic dipole-dipole interactions. Ultracold samples of dipolar molecules with long-range interactions offer a unique platform for quantum simulations and the study of correlated many-body physics. We provide an introduction to the physics of dipolar quantum gases, both electric and magnetic, and summarize the multipronged efforts to bring dipolar molecules into the quantum regime.…
We present a novel approach to precisely synthesize arbitrary polarization states of light with a high modulation bandwidth. Our approach consists of superimposing two laser light fields with the same wavelength, but with opposite circular polarizations, where the phase and the amplitude of each light field are individually controlled. We find that the polarization-synthesized beam reaches a degree of polarization of 99.99%, which is mainly limited by static spatial variations of the polarization state over the beam profile. We also find that the depolarization caused by temporal fluctuations …
We theoretically study collisions between ultracold polar molecules that are polarized by microwave or static electric fields. We systematically study the dependence on field strength, microwave polarization, and detuning from rotational transitions. We calculate the loss in two-body collisions that is observable experimentally and compare to the results expected for purely first-order dipolar interactions. For ground state molecules polarized by a static electric field, the dynamics are accurately described by first-order dipolar interactions. For microwave dressing, instead, resonant dipolar…
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 ma…
We demonstrate a scheme for direct absorption imaging of an ultracold ground-state polar molecular gas near quantum degeneracy. A challenge in imaging molecules is the lack of closed optical cycling transitions. Our technique relies on photon shot-noise limited absorption imaging on a strong bound-bound molecular transition. We present a systematic characterization of this imaging technique. Using this technique combined with time-of-flight (TOF) expansion, we demonstrate the capability to determine momentum and spatial distributions for the molecular gas. We anticipate that this imaging techn…
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 $^2Σ$ and $^1Σ$ 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 l…
We propose a new type of Feshbach resonance occurring when two different ultracold atoms in their ground state undergo an s-wave collision in the presence of a continuous-wave laser light. The atoms collide in the dissociation continuum of the molecular electronic ground state which is coupled by the light to a rovibrational level of the same electronic ground state: we name this a Laser-Assisted Self-Induced Feshbach Resonance (LASIFR). This mechanism, valid for all polar molecules, is analyzed on the example of ultracold 87Rb and 84Sr atoms, for which the laser frequency falls in the THz ran…
We study, both theoretically and experimentally, the dynamical polarizability $α(ω)$ of $\textrm{Rb}_2$ molecules in the rovibrational ground state of $\mathrm{a}^3Σ_u^+$. Taking all relevant excited molecular bound states into account, we compute the complex-valued polarizability $α(ω)$ for wave numbers up to $20000\:\textrm{cm}^{-1}$. Our calculations are compared to experimental results at $1064.5\:\textrm{nm}$ ($\sim9400\:\textrm{cm}^{-1}$) as well as at $830.4\:\textrm{nm}$ ($\sim12000\:\textrm{cm}^{-1}$). Here, we discuss the measurements at $1064.5\:\textrm{nm}$. The ultracold $\textrm{…
Progress in ultracold experiments with polar molecules requires a clear understanding of their interactions and reactivity at ultra-low collisional energies. Two important theoretical steps in this process are the characterization of interaction potentials between molecules and the modeling of reactive scattering mechanism. Here, we report on the {\it abinitio} calculation of isotropic and anisotropic van der Waals interaction potentials for polar KRb and RbCs colliding with each other or with ultracold atoms. Based on these potentials and two short-range scattering parameters we then develop …
We present a novel method for probing the alignment of the molecular axis of an ultracold, nonpolar dimer. These results are obtained using diatomic $^{87}\textrm{Rb}_2$ molecules in the vibrational ground state of the lowest triplet potential $a^3Σ_u^+$ trapped in a 3D optical lattice. We measure the molecular polarizabilities, which are directly linked to the alignment, along each of the $x$, $y$, and $z$ directions of the lab coordinate system. By preparing the molecules in various, precisely defined rotational quantum states we can control the degree of alignment of the molecular axis with…
Ultracold molecules trapped in optical tweezers show great promise for the implementation of quantum technologies and precision measurements. We study a prototypical scenario where two interacting polar molecules placed in separate traps are controlled using an external electric field. This, for instance, enables a quantum computing scheme in which the rotational structure is used to encode the qubit states. We estimate the typical operation timescales needed for state engineering to be in the range of few microseconds. We further underline the important role of the spatial structure of the tw…
Recently, the quest for an ultracold and dense ensemble of polar molecules has attracted strong interest. Polar molecules have bright prospects for novel quantum gases with long-range and anisotropic interactions, for quantum information science, and for precision measurements. However, high-density clouds of ultracold polar molecules have so far not been produced. Here, we report a key step towards this goal. Starting from an ultracold dense gas of heteronuclear 40K-87Rb Feshbach molecules with typical binding energies of a few hundred kHz and a negligible dipole moment, we coherently transfe…
We calculate pair potential curves for interacting Rydberg atoms in a constant electric field and use them to determine the effective $C_3$ dipole-dipole and $C_6$ van der Waals coefficients. We compare the $C_3$ and $C_6$ with experiments where the angle of a polarizing electric field is varied with respect to the axis of a quasi-1-dimensional trap at ultracold temperatures. The dipoles produced via polarization of the atoms have an angular dependent dipole-dipole interaction. We focus on the interaction potential of two rubidium Rydberg atoms in $50S_{1/2}$ states in the blockade regime. For…
We study the growth dynamics of ordered structures of strongly interacting polar molecules in optical lattices. Using dipole blockade of microwave excitations, we map the system onto an interacting spin-1/2 model possessing ground states with crystalline order, and describe a way to prepare these states by non-adiabatically driving the transitions between molecular rotational levels. The proposed technique bypasses the need to cross a phase transition and allows for the creation of ordered domains of considerably larger size compared to approaches relying on adiabatic preparation.
Arrays of trapped ultracold molecules represent a promising platform for implementing a universal quantum computer. DeMille has detailed a prototype design based on Stark states of polar $^1Σ$ molecules as qubits. Herein, we consider an array of polar $^2Σ$ molecules which are, in addition, inherently paramagnetic and whose Hund's case (b) free-rotor states are Bell states. We show that by subjecting the array to combinations of concurrent homogeneous and inhomogeneous electric and magnetic fields, the entanglement of the array's Stark and Zeeman states can be tuned and the qubit sites address…
