Starting from weakly bound Feshbach molecules, we demonstrate a two-photon pathway to the dipolar ground state of bi-alkali molecules that involves only singlet-to-singlet optical transitions. This pathway eliminates the search for a suitable intermediate state with sufficient singlet-triplet mixing and the exploration of its hyperfine structure, as is typical for pathways starting from triplet dominated Feshbach molecules. By selecting a Feshbach state with a stretched singlet hyperfine component and controlling the polarization of the excitation laser, we assure coupling to only a single hyperfine component of the $\textrm{A}^{1}Σ^{+}$ excited potential, even if the hyperfine structure is not resolved. Similarly, we address a stretched hyperfine component of the $\textrm{X}^{1}Σ^{+}$ rovibrational ground state, and therefore an ideal three level system is established. We demonstrate this pathway with ${}^{6}\textrm{Li}{}^{40}\textrm{K}$ molecules. By exploring deeply bound states of the $\textrm{A}^{1}Σ^{+}$ potential, we are able to obtain large and balanced Rabi frequencies for both transitions. This method can be applied to other molecular species.
In the mixture of ultracold spin-1 atoms of two different species A and B (e.g., $^{23}$Na (A) and $^{87}$Rb (B)), inter-species singlet-pairing process ${\rm A}_{+1}+{\rm B}_{-1}\rightleftharpoons {\rm A}_{-1}+{\rm B}_{+1}$, can be induced by the spin-dependent inter-atomic interaction, where subscript $\pm 1$ denotes the magnetic quantum number. Nevertheless, one cannot isolate this process from other spin-changing processes by tuning the bias real magnetic field. As a result, so far the singlet-pairing process have not been clearly observed in the experiments, and the measurement of the cor…
We report on high-resolution spectroscopy of ultracold fermionic \nak~Feshbach molecules, and identify a two-photon pathway to the rovibrational singlet ground state via a resonantly mixed \Bcres intermediate state. Photoassociation in a $^{23}$Na-$^{40}$K atomic mixture and one-photon spectroscopy on \nak~Feshbach molecules reveal about 20 vibrational levels of the electronically excited \ctrip state. Two of these levels are found to be strongly perturbed by nearby \Bsing states via spin-orbit coupling, resulting in additional lines of dominant singlet character in the perturbed complex {${\r…
We report on the formation of ultracold fermionic Feshbach molecules of $^{23}$Na$^{40}$K, the first fermionic molecule that is chemically stable in its ground state. The lifetime of the nearly degenerate molecular gas exceeds 100 ms in the vicinity of the Feshbach resonance. The measured dependence of the molecular binding energy on the magnetic field demonstrates the open-channel character of the molecules over a wide field range and implies significant singlet admixture. This will enable efficient transfer into the singlet vibrational ground state, resulting in a stable molecular Fermi gas …
The symmetry properties of the Cooper pairing problem for multi-component ultra-cold dipolar molecular systems are investigated. The dipolar anisotropy provides a natural and robust mechanism for both triplet and singlet Cooper pairing to first order in the interaction strength. With a purely dipolar interaction, the triplet $p_z$-like polar pairing is the most dominant. A short-range attractive interaction can enhance the singlet pairing to be nearly degenerate with the triplet pairing. We point out that these two pairing channels can mix by developing a relative phase of $\pm\fracπ{2}$, thus…
We report on the controlled creation of a valence bond state of delocalized effective-spin singlet and triplet dimers by means of a bichromatic optical superlattice. We demonstrate a coherent coupling between the singlet and triplet states and show how the superlattice can be employed to measure the singlet-fraction employing a spin blockade effect. Our method provides a reliable way to detect and control nearest-neighbor spin correlations in many-body systems of ultracold atoms. Being able to measure these correlations is an important ingredient to study quantum magnetism in optical lattices.…
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 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 spectroscopically investigate a pathway for the conversion of $^{23}\textrm{Na}^{39}\textrm{K}$ Feshbach molecules into rovibronic ground state molecules via STImulated Raman Adiabatic Passage (STIRAP). Using photoassociation spectroscopy from the diatomic scattering threshold in the $a^3Σ^+$ potential, we locate the resonantly mixed electronically excited intermediate states $|B^1Π, v=8\rangle$ and $|c^3Σ^+, v=30\rangle$ which, due to their singlet-triplet admixture, serve as an ideal bridge between predominantly $a^3Σ^+$ Feshbach molecules and pure $X^1Σ^+$ ground state molecules. We inve…
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 propose a scheme to investigate the interplay between Kondo-exchange interaction and quantum spin Hall effect with ultracold fermionic alkaline-earth atoms trapped in two-dimensional optical lattices using ultracold collision and laser-assisted tunneling. In the strong Kondo-coupling regime, though the loop trajectory of the mobile atom disappears, collective dynamics of an atom pair in two clock states can exhibit an unexpected spin-dependent cyclotron orbit in a plaquette, realizing the quantum spin Hall effect of the Kondo singlet. We demonstrate that the collective cyclotron dynamics of…
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…
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 investigate the competition of various exotic superfluid states in a chain of spin-polarized ultracold fermionic atoms with hyperfine spin $F = 3/2$ and s-wave contact interactions. We show that the ground state is an exotic inhomogeneous mixture in which two distinct superfluid phases --- spin-carrying pairs and singlet quartets --- form alternating domains in an extended region of the parameter space.
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 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.
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{…
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.
We report the creation of ultracold bosonic $^{23}$Na$^{87}$Rb Feshbach molecules via magneto-association. By ramping the magnetic field across an interspecies Feshbach resonance, at least 4000 molecules can be produced out of the near degenerate ultracold mixture. Fast loss due to inelastic atom-molecule collisions is observed, which limits the pure molecule number, after residual atoms removal, to 1700. The pure molecule sample can live for 21.8(8) ms in the optical trap, long enough for future molecular spectroscopy studies toward coherently transferring to the singlet ro-vibrational ground…
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…
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 …
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…
We show that radiofrequency (RF) radiation may be used to create Feshbach resonances in ultracold gases of alkali-metal atoms at desired magnetic fields that are convenient for atomic cooling and degeneracy. For the case of $^{39}$K+$^{133}$Cs, where there are no RF-free resonances in regions where Cs may be cooled to degeneracy, we show that a resonance may be created near 21~G with 69.2~MHz RF radiation. This resonance is almost lossless with circularly polarized RF, and the molecules created are long-lived even with plane-polarized RF.
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…
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…
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.
We present a technique for engineering quantum magnets via ultracold polar molecules in optical lattices and explore exotic interplay between its spin superfluidity and solidity. The molecular ground and first excited rotational states are resonantly coupled by a linearly polarized microwave field. The spin-up (spin-down) states are presented by molecular rotational states of electric dipole moment along (against) the coupling field. By controlling the angle between the lattice direction and the coupling field, the inter-site interaction can be tuned from antiferromagnetic to ferromagnetic. Fu…
The dynamics of a bilayer system of ultracold dipolar molecules exhibits classical and quantum glassy behavior, characterized by long tails in the relaxation time and dynamical heterogeneity. In the proposed setup, quantum fluctuations are of the order of thermal fluctuations and the degree of frustration can tuned by the interlayer distance. We present experimental accessible order parameters based on marker molecules, distinguished by properly chosen internal levels, and find quantum features of dynamical heterogeneity.
Ultracold polar molecules offer the possibility of exploring quantum gases with interparticle interactions that are strong, long-range, and spatially anisotropic. This is in stark contrast to the dilute gases of ultracold atoms, which have isotropic and extremely short-range, or "contact", interactions. The large electric dipole moment of polar molecules can be tuned with an external electric field; this provides unique opportunities such as control of ultracold chemical reactions, quantum information processing, and the realization of novel quantum many-body systems. In spite of intense exper…
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…
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-reso…
In this review, we discuss the properties of a few impurity atoms immersed in a gas of ultracold fermions, the so-called Fermi polaron problem. On one side, this many-body system is appealing because it can be described almost exactly with simple diagrammatic and/or variational theoretical approaches. On the other, it provides quantitatively reliable insight into the phase diagram of strongly interacting population imbalanced quantum mixtures. In particular, we show that the polaron problem can be applied to study itinerant ferromagnetism, a long standing problem in quantum mechanics.
Recent work on ultracold polar molecules, governed by a generalization of the t-J Hamiltonian, suggests that molecules may be better suited than atoms for studying d-wave superfluidity due to stronger interactions and larger tunability of the system. We compute the phase diagram for polar molecules in a checkerboard lattice consisting of weakly coupled square plaquettes. In the simplest experimentally realizable case where there is only tunneling and an XX-type spin-spin interaction, we identify the parameter regime where d-wave superfluidity occurs. We also find that the inclusion of a densit…
We explore the feasibility of optically forming long-range tetratomic and larger polyatomic molecules in their ground electronic state from ultracold pairs of polar molecules aligned by external fields. Depending on the relative orientation of the interacting diatomic molecules, we find that a tetratomic can be formed either as a weakly bound complex in a very extended halo state or as a pure long-range molecule composed of collinear or nearly-collinear diatomic molecules. The latter is a novel type of tetratomic molecule comprised of two diatomic molecules bound at long intermolecular range a…
We report on two-photon photoassociation (PA) spectroscopy of ultracold heteronuclear LiRb molecules. This is used to determine the binding energies of the loosely bound levels of the electronic ground singlet and the lowest triplet states of LiRb. We observe strong two-photon PA lines with power broadened line widths greater than 20 GHz at relatively low laser intensity of 30 W/cm$^{2}$. The implication of this observation on direct atom to molecule conversion using stimulated Raman adiabatic passage (STIRAP) is discussed and the prospect for electronic ground state molecule production is the…
Ultracold atoms and molecules trapped in optical lattices are expected to serve as simulators of strongly correlated systems and topological states of matter. A fascinating example is to realize the Kitaev quantum spin liquid by using ultracold polar molecules. However, although experimental implementation of the Kitaev-type interaction was proposed, the stability of the Kitaev quantum spin liquid has not been fully investigated thus far. Here we study a quantum spin model with long-range angle-dependent Kitaev-type interactions proposed for the polar molecules, by the pseudofermion functional…
We present and analyze a toolbox for the controlled manipulation of ultracold polar molecules, consisting of detection of molecules, atom-molecule entanglement, and engineering of dissipative dynamics. Our setup is based on fast chemical reactions between molecules and atoms leading to a quantum Zeno-based collisional blockade in the system. We demonstrate that the experimental parameters for achieving high fidelities can be found using a straightforward numerical optimization. We exemplify our approach for a system comprised of NaK molecules and Na atoms and we discuss the consequences of res…
The system of ultracold atoms with hyperfine spin $F=3/2$ might be unstable against the formation of quintet pairs if the interaction is attractive in the quintet channel. We have investigated the behavior of correlation functions in a model including only s-wave interactions at quarter filling by large-scale density-matrix renormalization-group simulations. We show that the correlations of quintet pairs become quasi-long-ranged, when the system is partially polarized, leading to the emergence of various mixed superfluid phases in which BCS-like pairs carrying different magnetic moment coexist…
We show that single-component fermionic polar molecules confined to a 2D geometry and dressed by a microwave field, may acquire an attractive $1/r^3$ dipole-dipole interaction leading to superfluid p-wave pairing at sufficiently low temperatures even in the BCS regime. The emerging state is the topological $p_x+ip_y$ phase promising for topologically protected quantum information processing. The main decay channel is via collisional transitions to dressed states with lower energies and is rather slow, setting a lifetime of the order of seconds at 2D densities $\sim 10^8$ cm$^{-2}$.
An impurity atom immersed in an ultracold atomic Fermi gas can form a quasiparticle, so-called Fermi polaron, due to impurity-fermion interaction. We consider a three-dimensional homogeneous dipolar Fermi gas as a medium, where the interatomic dipole-dipole interaction (DDI) makes the Fermi surface deformed into a spheroidal shape, and, using a Chevy-type variational method, investigate the ground-state properties of the Fermi polaron: the effective mass, the momentum distribution of a particle-hole (p-h) excitation, the drag parameter, and the medium density modification around the impurity. …
By selecting two dressed rotational states of ultracold polar molecules in an optical lattice, we obtain a highly tunable generalization of the t-J model, which we refer to as the t-J-V-W model. In addition to XXZ spin exchange, the model features density-density interactions and novel density-spin interactions; all interactions are dipolar. We show that full control of all interaction parameters in both magnitude and sign can be achieved independently of each other and of the tunneling. As a first step towards demonstrating the potential of the system, we apply the density matrix renormalizat…
Recent theory has indicated how to emulate tunable models of quantum magnetism with ultracold polar molecules. Here we show that present molecule optical lattice experiments can accomplish three crucial goals for quantum emulation, despite currently being well below unit filling and not quantum degenerate. The first is to verify and benchmark the models proposed to describe these systems. The second is to prepare correlated and possibly useful states in well-understood regimes. The third is to explore many-body physics inaccessible to existing theoretical techniques. Our proposal relies on a n…
We present a unified formalism for describing chemical reaction rates of trapped, ultracold molecules. This formalism reduces the scattering to its essential features, namely, a propagation of the reactant molecules through a gauntlet of long-range forces before they ultimately encounter one another, followed by a probability for the reaction to occur once they do. In this way, the electric-field dependence should be readily parametrized in terms of a pair of fitting parameters (along with a $C_6$ coefficient) for each asymptotic value of partial wave quantum numbers $|L,M \rangle$. From this,…
We investigate the BCS pairing in a mixture of fermionic polar molecules with two different hyperfine states. We derive a set of coupled gap equations and find that this system supports both spin-singlet and -triplet BCS pairs. We also calculate the critical temperatures and the angular dependence of order parameters. In addition, by tuning short-range interaction between inter-species molecules, the transition between singlet and triplet paired states may be realized.
We report on the creation of an ultracold dipolar gas of fermionic $^{23}$Na$^{40}$K molecules in their absolute rovibrational and hyperfine ground state. Starting from weakly bound Feshbach molecules, we demonstrate hyperfine resolved two-photon transfer into the singlet ${\rm X}^1Σ^+ |v{=}0,J{=}0\rangle$ ground state, coherently bridging a binding energy difference of 0.65 eV via stimulated rapid adiabatic passage. The spin-polarized, nearly quantum degenerate molecular gas displays a lifetime longer than 2.5 s, highlighting NaK's stability against two-body chemical reactions. A homogeneous …
