A recent experiment reported for the first time the preparation of a Fermi degenerate gas of polar molecules and observed a suppression of their chemical reaction rate compared to the one expected from a purely classical treatment. While it was hypothesized that the suppression in the ultracold regime had its roots in the Fermi statistics of the molecules, this argument is inconsistent with the fact that the Fermi pressure should set a lower bound for the chemical reaction rate. Therefore it can not be explained from standard two-body $p$-wave inelastic collisions. Here we develop a simple model of chemical reactions that occur via the formation and decay of molecular complexes. We indeed find that pure two-body molecule losses are unable to explain the observed suppression. Instead we extend our description beyond two-body physics by including effective complex-molecule interactions possible emerging from many-body and effective medium effects at finite densities and in the presence of trapping light. %Under this framework we observe that additional complex-molecule collisions, which manifest as a net three-body molecular interaction could give rise to the additional suppression. Although our effective model is able to quantitatively reproduce recent experimental observations, a detailed understanding of the actual physical mechanism responsible for these higher-order interaction processes is still pending.
Quantum degenerate molecules represent a new paradigm for fundamental studies and practical applications. Association of already quantum degenerate atoms into molecules provides a crucial shortcut around the difficulty of cooling molecules to ultracold temperatures. Whereas association can be induced with either laser or magnetic fields, photoassociation requires impractical laser intensity to overcome poor overlap between the atom pair and molecular wavefunctions, and experiments are currently restricted to magnetoassociation. Here we model realistic production of a quantum degenerate gas of …
A recent experimental realization of quantum degenerate gas of $^{40}$K$^{87}$Rb molecules opens up prospects of exploring strong dipolar Fermi gases and many-body phenomena arising in that regime. Here we derive a mean-field variational approach based on the Wigner function for the description of ground-state properties of such systems. We show that the stability of dipolar fermions in a general harmonic trap is universal as it only depends on the trap aspect ratios and the dipoles' orientation. We calculate the species-independent stability diagram and the deformation of the Fermi surface (F…
First-order phase transition in atom-molecule quantum degenerate mixtures with coherent three-body recombination
Missouri University of Science and Technology（密苏里科技大学）；Ben-Gurion University of the Negev（内盖夫本古里安大学）；Harvard & Smithsonian（哈佛大学与史密森尼学会）；University of Chicago（芝加哥大学）
It has long been expected that quantum degenerate gases of molecules would open access to a wide range of phenomena in molecular and quantum sciences. However, the very complexity that makes ultracold molecules so enticing has made reaching degeneracy an outstanding experimental challenge over the past decade. We now report the production of a Fermi degenerate gas of ultracold polar molecules of potassium--rubidium (KRb). Through coherent adiabatic association in a deeply degenerate mixture of a rubidium Bose-Einstein condensate and a potassium Fermi gas, we produce molecules at temperatures b…
We present the essential experimental steps of our all-optical approach to prepare a double-degenerate Fermi-Fermi mixture of 6Li and 40K atoms, which then serves as a starting point for molecule formation. We first describe the optimized trap loading procedures, the internal-state preparation of the sample, and the combined evaporative and sympathetic cooling process. We then discuss the preparation of the sample near an interspecies Feshbach resonance, and we demonstrate the formation of heteronuclear molecules by a magnetic field ramp across the resonance.
We present a method to design a finite decay rate for excited rotational states in polar molecules. The setup is based on a hybrid system of polar molecules with atoms driven into a Rydberg state. The atoms and molecules are coupled via the strong dipolar exchange interaction between two rotation levels of the polar molecule and two Rydberg states. Such a controllable decay rate opens the way to optically pump the hyperfine levels of polar molecules and it enables the application of conventional laser cooling techniques for cooling polar molecules into quantum degeneracy.
We report on the preparation of a quantum degenerate mixture of $^{23}$Na$^{40}$K molecules and $^{40}$K atoms. A deeply degenerate atomic mixture of $^{23}$Na and $^{40}$K atoms with a large number ratio ($N_F/N_B\approx 6$) is prepared by the mode-matching loading of atoms from a cloverleaf-type magnetic trap into a large-volume horizontal optical dipole trap and evaporative cooling in a large-volume three-beam optical dipole trap. About $3.0\times10^4$ $^{23}$Na$^{40}$K ground-state molecules are created through magneto-association followed by stimulated adiabatic Raman passage. The 2D dens…
In this work we demonstrate a dynamic process in which SO coupling can coherently produce s-wave Feshbach molecules from a fully polarized Fermi gas, and can induce a coherent oscillation between Feshbach molecules and spin polarized gas. For comparison, we also show that such phenomena are absent if the inter-component coupling is momentum-independent. This demonstrates experimentally that SO coupling does provide finite matrix element between a singlet state and a triplet state, and therefore, implies the bound pairs of a system with SO coupling have triplet p-wave component, which can becom…
We realize a non-degenerate two-mode Dicke model with competing interactions in a Bose-Einstein condensate (BEC) coupled to two orthogonal polarization modes of a single optical cavity. The BEC is coupled to the cavity modes via the scalar and vectorial part of the atomic polarizability. We can independently change these couplings and determine their effect on a self-organization phase transition. Measuring the phases of the system, we characterize a crossover from a single-mode to a two-mode Dicke model. This work provides perspectives for the realization of coupled phases of spin and density…
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 ground state and spectral properties of Bose gases in double-well potentials are studied in two different scenarios: i) an interacting atomic Bose gas, and ii) a mixture of an atomic gas interacting with diatomic molecules. A ground state second-order quantum phase transition (QPT) is observed in both scenarios. For large attractive values of the atom-atom interaction, the ground-state is degenerate. For repulsive and small attractive interaction, the ground-state is not degenerate and is well approximated by a boson coherent state. Both systems depict an excited state quantum phase transi…
We study a system of polar dipolar fermions in a two-dimensional optical lattice and show that multi-band Fermi-Hubbard model is necessary to discuss such system. By taking into account both on-site, and long-range interactions between different bands, as well as occupation-dependent inter- and intra-band tunneling, we predict appearance of novel phases in the strongly-interacting limit.
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 observe thermalization in the production of a degenerate Fermi gas of polar ${}^{40}\text{K}{}^{87}\text{Rb}$ molecules. By measuring the atom--dimer elastic scattering cross section near the Feshbach resonance, we show that Feshbach molecules rapidly reach thermal equilibrium with both parent atomic species. Equilibrium is essentially maintained through coherent transfer to the ground state. Sub-Poissonian density fluctuations in Feshbach and ground-state molecules are measured, giving an independent characterization of degeneracy and directly probing the molecular Fermi--Dirac distributio…
We revisit the polaron-molecule transition in three-dimensional(3D) fermion systems using the well-established variational approach. The molecule is found to be intrinsically unstable against lowest-order particle-hole excitations, and it can only approximate the ground state of impurity system with finite total momentum in the strong coupling regime. The polaron-molecule transition can therefore be reinterpreted as a first-order transition between single impurity systems with different total momenta. Within certain interaction window near their transition, both states appear as local minima i…
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 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 show that recently suggested subwavelength lattices offer remarkable prospects for the observation of novel superfluids of fermionic polar molecules. It becomes realistic to obtain a topological $p$-wave superfluid of microwave-dressed polar molecules in 2D lattices at temperatures of the order of tens of nanokelvins, which is promising for topologically protected quantum information processing. Another foreseen novel phase is an interlayer $p$-wave superfluid of polar molecules in a bilayer geometry.
Ultracold polar molecules are an ideal platform for studying many-body physics with long-range dipolar interactions. Experiments in this field have progressed enormously, and several groups are pursuing advanced apparatus for manipulation of molecules with electric fields as well as single-atom-resolved in situ detection. Such detection has become ubiquitous for atoms in optical lattices and tweezer arrays, but has yet to be demonstrated for ultracold polar molecules. Here we present a proposal for the implementation of quantum gas microscopy for polar molecules, and specifically discuss a tec…
The observation of significant dipolar effects in gases of ultra-cold polar molecules typically demands a strong external electric field to polarize the molecules. We show that even in the absence of a significant polarization, dipolar effects may play a crucial role in the physics of polar molecules in bilayers, provided that the molecules in each layer are initially prepared in a different rotational state. Then, inter-layer dipolar interactions result in a non-local swap of the rotational state between molecules in different layers, even for weak applied electric fields. The inter-layer sca…
Polar molecules in geometrically frustrated lattices may result in a very rich landscape of quantum phases, due to the non-trivial interplay between frustration, and two- and possibly three-body inter-site interactions. In this paper, we illustrate this intriguing physics for the case of hard-core polar molecules in frustrated triangular ladders. Whereas commensurate lattice fillings result in gapped phases with bond-order and/or density-wave order, at incommensurate fillings we find chiral-, two-component-, and pair-superfluids. We show as well that, remarkably, polar molecules in frustrated …
The spectrum of collective excitations of degenerate partially polarized spin-1/2 fermions is considered. The spin-up fermions and the spin-down fermions are considered as different fluids. Corresponding two-fluid hydrodynamics consistent with a non-linear Pauli equation is suggested. An equation of state for the spin current caused by the distribution of particles on different energy levels is suggested for the degenerate regime, where the spin current is caused by the Pauli blocking. Spectrum of three waves is found as a solution of the hydrodynamic equations: two sound waves and one spin wa…
We propose a scheme to realize a pseudospin-$1/2$ model of the $^{1}Σ(v=0)$ bialkali polar molecules with the spin states corresponding to two sublevels of the first excited rotational level. We show that the effective dipole-dipole interaction between two spin-$1/2$ molecules couples the rotational and orbital angular momenta and is highly tunable via a microwave field. We also investigate the ground state properties of a spin-$1/2$ molecular condensate. A variety of nontrivial quantum phases, including the doubly-quantized vortex states, are discovered. Our scheme can also be used to create …
We investigate novel f-wave superfluids of fermionic polar molecules in a two-dimensional bilayer system with dipole moments polarized perpendicular to the layers and in opposite directions in different layers. The solution of the BCS gap equation reveals that these unconventional superfluids emerge at temperatures on the level of femtokelvin which opens up new possibilities to explore the topological f+i f phase, quantum interferometry and Majorana fermions in experiments with ultracold polar molecules. The experimental realization of such interesting novel f-wave pairings is discussed.
The association process of Feshbach molecules is well described by a Landau-Zener (LZ) transition above the Fermi temperature, such that two-body physics dominates the dynamics. However, using $^6$Li atoms and the associated Feshbach resonance at $B_r=834.1$ G, we observe an enhancement of the atom-molecule coupling as the fermionic atoms reach degeneracy, demonstrating the importance of many-body coherence not captured by the conventional LZ model. In the experiment, we apply a linear association ramp ranging from adiabatic to non-equilibrium molecule association for various temperatures. We …
The ground state of an impurity immersed in a Fermi sea changes from a polaron to a molecule as the interaction strength is increased. We show here that the coupling between these two states is strongly suppressed due to a combination of phase space effects and Fermi statistics, and that it vanishes much faster than the energy difference between the two states, thereby confirming the first order nature of the polaron-molecule transition. In the regime where each state is metastable, we find quasiparticle lifetimes which are much longer than what is expected for a usual Fermi liquid. Our analys…
Using exact Bethe ansatz (BA) solutions, we show that a spin-down fermion immersed into a fully polarized spin-up Fermi sea with a weak attraction is dressed by the surrounding spin-up fermions to form the one-dimensional analog of a polaron. As the attraction becomes strong, the spin-down fermion binds with one spin-up fermion to form a tightly bound molecule. Throughout the whole interaction regime, a crossover from the polaron to a molecule state is fully demonstrated through exact results of the excitation spectrum, the effective mass, binding energy and kinetic energy. Furthermore, a clea…
We consider an oblate Bose-Einstein condensate of heteronuclear polar molecules in a weak applied electric field. This system supports a rich quasiparticle spectrum that plays a critical role in determining its bulk dielectric properties. In particular, in sufficiently weak fields the system undergoes a polarization wave rotonization, leading to the development of textured electronic structure and a dielectric instability that is characteristic of the onset of a negative static dielectric function.
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.
Two-photon-assisted collisions in ultracold gases of polar molecules II : Optical shielding of ultracold polar molecular collisions
Université Paris-Saclay（巴黎萨克雷大学）；CNRS（法国国家科学研究中心）；Laboratoire Aimé Cotton（安伯特实验室）；Université Bourgogne Europe（勃艮第欧洲大学）；Laboratoire Interdisciplinaire Carnot de Bourgogne ICB UMR 6303（勃艮第卡诺跨学科实验室）；Institut für Quantenoptik, Leibniz Universität Hannover（汉诺威莱布尼茨大学量子光学研究所）
Understanding the behavior of an impurity strongly interacting with a Fermi sea is a long-standing challenge in many-body physics. When the interactions are short-ranged, two vastly different ground states exist: a polaron quasiparticle and a molecule dressed by the majority atoms. In the single-impurity limit, it is predicted that at a critical interaction strength, a first-order transition occurs between these two states. Experiments, however, are always conducted in the finite temperature and impurity density regime. The fate of the polaron-to-molecule transition under these conditions, whe…
The exploration of cold polar molecules in different geometries is a rapidly developing experimental and theoretical pursuit. Recently, the implementation of optical lattices has enabled confinement in stacks of planes, the number of which is also controllable. Here we consider the bound state structure of two polar molecules confined in two adjacent planes as function of the polarization angle of the dipole moment of the molecules. We prove analytically and present numerical evidence for the existence of bound states for arbitrary dipole moments and polarization directions in this two-dimensi…
We analyze a system of polar molecules in a one-dimensional optical lattice. By controlling the internal structure of the polar molecules with static electric and microwave fields, we demonstrate the appearance of a quantum phase transition into a ferroelectric phase via spontaneous breaking of a $U(1)$ symmetry. The phase diagram is first analyzed within mean-field theory, while in a second step the results are verified by a mapping onto the Bose-Hubbard model for hard-core bosons. The latter is studied within the well-established bosonization procedure. We find that the ferroelectric phase i…
We consider fermionic polar molecules in a bilayer geometry where they are oriented perpendicularly to the layers, which permits both low inelastic losses and superfluid pairing. The dipole-dipole interaction between molecules of different layers leads to the emergence of interlayer superfluids. The superfluid regimes range from BCS-like fermionic superfluidity with a high $T_c$ to Bose-Einstein (quasi-)condensation of interlayer dimers, thus exhibiting a peculiar BCS-BEC crossover. We show that one can cover the entire crossover regime under current experimental conditions.
We study unconventional superfluids of fermionic polar molecules in a two-dimensional bilayer system with dipoles are head-to-tail across the layers. We analyze the critical temperature of several unconventional pairings as a function of different system parameters. The peculiar competition between the $d$- and the $s$- wave pairings is discussed. We show that the experimental observation of such unconventional superfluids requires ulralow temperatures, which opens up new possibilities to realize several topological phases.
An experimental proposal for realizing spin-orbit (SO) coupling of pseudospin-1 in the ground manifold $^1Σ(\upsilon=0)$ of (bosonic) bialkali polar molecules is presented. The three spin components are composed of the ground rotational state and two substates from the first excited rotational level. Using hyperfine resolved Raman processes through two select excited states resonantly coupled by a microwave, an effective coupling between the spin tensor and linear momentum is realized. The properties of Bose-Einstein condensates for such SO-coupled molecules exhibiting dipolar interactions are…
Quantum degenerate cold-atom gases provide a remarkable opportunity to study strongly interacting systems. Recent experimental progress in producing ultracold polar molecules with a net electric dipole moment opens up new possibilities to realize novel quantum phases governed by the long-range and anisotropic dipole-dipole interactions. In this work we predict the existence of experimentally observable novel broken-symmetry states with spontaneous interlayer coherence in cold polar molecules. These exotic states appear due to strong repulsive interlayer interactions and exhibit properties of s…
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.
We study the spectrum of an impurity coupled to a Fermi sea (e.g., minority atom in an ultracold gas, exciton in a solid) by attraction strong enough to form a molecule/trion. We introduce a diagrammatic scheme which allows treating a finite mass impurity while reproducing the Fermi edge singularity in the immobile limit. For large binding energies the spectrum is characterized by a semi-coherent repulsive polaron and an incoherent molecule-hole continuum, which is the lowest-energy feature in the single-particle spectrum. The previously predicted attractive polaron seems not to exist for stro…
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 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 …
Superpositions of rotational states in polar molecules induce strong, long-range dipolar interactions. Here we extend the rotational coherence by nearly one order of magnitude to 8.7(6) ms in a dilute gas of polar $^{23}$Na$^{40}$K molecules in an optical trap. We demonstrate spin-decoupled magic trapping, which cancels first-order and reduces second-order differential light shifts. The latter is achieved with a dc electric field that decouples nuclear spin, rotation and trapping light field. We observe density-dependent coherence times, which can be explained by dipolar interactions in the bu…
We propose a method for sensitive parallel detection of low-frequency electromagnetic fields based on the fine structure interactions in paramagnetic polar molecules. Compared to the recently implemented scheme employing ultracold $^{87}$Rb atoms [B{ö}hi \textit{et al.}, Appl. Phys. Lett. \textbf{97}, 051101 (2010)], the technique based on molecules offers a 100-fold higher sensitivity, the possibility to measure both the electric and magnetic field components, and a probe of a wide range of frequencies from the dc limit to the THz regime.
Low-energy two-dimensional scattering is particularly sensitive to the existence and properties of weakly-bound states. We show that interaction potentials $V(r)$ with vanishing zero-momentum Born approximation $\int d^2r V(r)=0$ lead to an anomalously weak bound state which crucially modifies the two-dimensional scattering properties. This anomalous case is especially relevant in the context of polar molecules in bilayer arrangements.
We show that dressing polar molecules with a far-off-resonant optical field leads to new types of intermolecular potentials, which undergo a crossover from the inverse-power to oscillating behavior depending on the intermolecular distance, and whose parameters can be tuned by varying the laser intensity and wavelength. We present analytic expressions for the potential energy surfaces, thereby providing direct access to the parameters of an optical field required to design intermolecular interactions experimentally.
