Application of lasers to ultracold atoms and molecules
Hélène Perrin, Pierre Lemonde, Franck Pereira Dos Santos, Vincent Josse, Bruno Laburthe-Tolra, Frédéric Chevy, Daniel Comparat
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Review paper written in the name of IFRAF to celebrate 50 years of lasers and their applications to cold atom physics; 15 pages, 2 figures; to appear in Comptes Rendus de l'Academie des Sciences, Paris
In this review, we discuss the impact of the development of lasers on ultracold atoms and molecules and their applications. After a brief historical review of laser cooling and Bose-Einstein condensation, we present important applications of ultra cold atoms, including time and frequency metrology, atom interferometry and inertial sensors, atom lasers, simulation of condensed matter systems, production and study of strongly correlated systems, and production of ultracold molecules.
We study the dissociation of Feshbach molecules in ultracold Fermi gases with spin-orbit (SO) coupling. Since SO coupling can induce quantum transition between the Feshbach molecules and the fully polarized Fermi gas, the Feshbach molecules can be dissociated by the SO coupling. We experimentally realized this new type of dissociation in ultracold gases of 40K atoms with SO coupling created by Raman beams, and observed that the dissociation rate is highly non-monotonic on both the positive and negative Raman-detuning sides. Our results show that the dissociation of Feshbach molecules can be co…
We show that conical intersections can be created in laboratory coordinates by dressing a parabolic trap for ultracold atoms or molecules with a combination of optical and static magnetic fields. The resulting ring trap can support single-particle states with half-integer rotational quantization and many-particle states with persistent flow. Two well-separated atomic or molecular states are brought into near-resonance by an optical field and tuned across each other with an inhomogeneous magnetic field. Conical intersections occur at the nodes in the optical field.
We present first results on our implementation of a laser based accelerator for ultracold atoms. Atoms cooled to a temperature of 420 nK are confined and accelerated by means of laser tweezer beams and the atomic scattering is directly observed in laser absorption imaging. The optical collider has been characterized using Rb87 atoms in the |F=2,mF=2> state, but the scheme is not restricted to atoms in any particular magnetic substates and can readily be extended to other atomic species as well.
The realization of ultracold polar molecules in laboratories has pushed both physics and chemistry to new realms. In particular, these polar molecules offer scientists unprecedented opportunities to explore chemical reactions in the ultracold regime where quantum effects become profound. However, a key question about how two-body losses depend on quantum correlations in an interacting many-body system remains open so far. Here, we present a number of universal relations that directly connect two-body losses to other physical observables, including the momentum distribution and density correlat…
We produce an ultracold and dense sample of rovibronic ground state Cs_2 molecules close to the regime of quantum degeneracy, in a single hyperfine level, in the presence of an optical lattice. The molecules are individually trapped, in the motional ground state of an optical lattice well, with a lifetime of 8 s. For preparation, we start with a zero-temperature atomic Mott-insulator state with optimized double-site occupancy and efficiently associate weakly-bound dimer molecules on a Feshbach resonance. Despite extremely weak Franck-Condon wavefunction overlap, the molecules are subsequently …
We derive effective lattice models for ultracold bosonic or fermionic nonreactive molecules (NRMs) in an optical lattice, analogous to the Hubbard model that describes ultracold atoms in a lattice. In stark contrast to the Hubbard model, which is commonly assumed to accurately describe NRMs, we find that the single on-site interaction parameter $U$ is replaced by a multi-channel interaction, whose properties we elucidate. The complex, multi-channel collisional physics is unrelated to dipolar interactions, and so occurs even in the absence of an electric field or for homonuclear molecules. We f…
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…
We report the creation of ultracold bosonic dipolar $^{23}\textrm{Na}^{39}\textrm{K}$ molecules in their absolute rovibrational ground state. Starting from weakly bound molecules immersed in an ultracold atomic mixture, we coherently transfer the dimers to the rovibrational ground state using an adiabatic Raman passage. We analyze the two-body decay in a pure molecular sample and in molecule-atom mixtures and find an unexpectedly low two-body decay coefficient for collisions between molecules and $^{39}\textrm{K}$ atoms in a selected hyperfine state. The preparation of bosonic $^{23}\textrm{Na…
The creation of ultracold molecules is currently limited to diatomic species. In this letter we present a theoretical description of the photoassociation of ultracold atoms and molecules to create ultracold excited triatomic molecules, thus being a novel example of light-assisted ultracold chemical reaction. The calculation of the photoassociation rate of ultracold Cs atoms with ultracold Cs$_2$ molecules in their rovibrational ground state is reported, based on the solution of the quantum dynamics involving the atom-molecule long-range interactions, and assuming a model potential for the shor…
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.
The quantum mechanical few-body problem at ultracold energies poses severe challenges to theoretical techniques, particularly when long-range interactions are present that decay only as a power-law potential. In this paper we review the techniques and progress in studies of universal few-body physics for ultracold atoms, particularly those related to long-range interactions.
Harnessing the potential wide-ranging quantum science applications of molecules will require control of their interactions. Here, we use microwave radiation to directly engineer and tune the interaction potentials between ultracold calcium monofluoride (CaF) molecules. By merging two optical tweezers, each containing a single molecule, we probe collisions in three dimensions. The correct combination of microwave frequency and power creates an effective repulsive shield, which suppresses the inelastic loss rate by a factor of six, in agreement with theoretical calculations. The demonstrated mic…
Arrays of single ultracold molecules promise to be a powerful platform for many applications ranging from quantum simulation to precision measurement. Here we report on the creation of an optical tweezer array of single ultracold CaF molecules. By utilizing light-induced collisions during the laser cooling process, we trap single molecules. The high densities attained inside the tweezer traps have also enabled us to observe in the absence of light molecule-molecule collisions of laser cooled molecules for the first time.
We describe the formation of fermionic NaLi Feshbach molecules from an ultracold mixture of bosonic 23Na and fermionic 6Li. Precise magnetic field sweeps across a narrow Feshbach resonance at 745 G result in a molecule conversion fraction of 5% for our experimental densities and temperatures, corresponding to a molecule number of 5*10^4. The observed molecular decay ifetime is 1.3 ms after removing free Li and Na atoms from the trap.
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 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…
We report the observation of a dimer-dimer inelastic collision resonance for ultracold Feshbach molecules made of bosonic sodium and rubidium atoms. This resonance, which we attribute to the crossing of the dimer-dimer threshold with a heteronuclear tetramer state, manifests itself as a pronounced inelastic loss peak of dimers when the interspecies scattering length between the constituent atoms is tuned. Near this resonance, a strong modification of the temperature dependence of the dimer-dimer scattering is observed. Our result provides insight into the heteronuclear four-body system consist…
We measure inelastic collisions between ultracold CaF molecules by combining two optical tweezers, each containing a single molecule. We observe collisions between $^2Σ$ CaF molecules in the absolute ground state $|X,v=0, N=0,F=0\rangle$, and in excited hyperfine and rotational states. In the absolute ground state, we find a two-body loss rate of $7(4) \times 10^{-11} \text{cm}^{3}/\text{s}$, which is below, but close to the predicted universal loss rate.
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 lo…
In a combined experimental and theoretical effort, we demonstrate a novel type of dipolar system made of ultracold bosonic dipolar molecules with large magnetic dipole moments. Our dipolar molecules are formed in weakly bound Feshbach molecular states from a sample of strongly magnetic bosonic erbium atoms. We show that the ultracold magnetic molecules can carry very large dipole moments and we demonstrate how to create and characterize them, and how to change their orientation. Finally, we confirm that the relaxation rates of molecules in a quasi-two dimensional geometry can be reduced by usi…
This article gives an introduction to the realization of effective quantum magnetism with ultracold molecules in an optical lattice, reviews experimental and theoretical progress, and highlights future opportunities opened up by ongoing experiments. Ultracold molecules offer capabilities that are otherwise difficult or impossible to achieve in other effective spin systems, such as long-ranged spin-spin interactions with controllable degrees of spatial and spin anisotropy and favorable energy scales. Realizing quantum magnetism with ultracold molecules provides access to rich many-body behavior…
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 …
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 present investigations of the formation rate and collisional stability of lithium Feshbach molecules in an ultracold three-component mixture composed of two resonantly interacting fermionic 6-Li spin states and bosonic 174-Yb. We observe long molecule lifetimes (> 100 ms) even in the presence of a large ytterbium bath and extract reaction rate coefficients of the system. We find good collisional stability of the mixture in the unitary regime, opening new possibilities for studies and probes of strongly interacting quantum gases in contact with a bath species.
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 the full control over the internal states of ultracold $^{23}$Na$^{87}$Rb molecules, including vibrational, rotational and hyperfine degrees of freedom. Starting from a sample of weakly bound Feshbach molecules, we realize the creation of molecules in single hyperfine levels of both the rovibrational ground and excited states with a high-efficiency and high-resolution stimulated Raman adiabatic passage. Starting from the rovibrational and hyperfine ground state, we demonstrate rotational and hyperfine control with one- and two-photon microwave spectroscopy. This achievement of fully …
We report the successful production of an ultracold sample of absolute ground-state $^{23}$Na$^{87}$Rb molecules. Starting from weakly-bound Feshbach molecules formed via magneto-association, the lowest rovibrational and hyperfine level of the electronic ground state is populated following a high efficiency and high resolution two-photon Raman process. The high purity absolute ground-state samples have up to 8000 molecules and densities of over $10^{11}$ cm$^{-3}$. By measuring the Stark shifts induced by external electric fields, we determined the permanent electric dipole moment of the absol…
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.…
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…
Photoassociation (PA) is a powerful technique to synthesize molecules directly and continuously from cold and ultracold atoms into deeply bound molecular states. In freespace, however, PA efficiency is constrained by the number of spontaneous decay channels linking the initial excited molecular state to a sea of final (meta)stable rovibronic levels. Here, we propose a novel scheme based on molecules strongly coupled to a guided photonic mode in a photonic crystal waveguide that turns PA into a powerful tool for near deterministic formation of ultracold molecules in their ground rovibrational l…
Measuring the statistical correlations of individual quantum objects provides an excellent way to study complex quantum systems. Ultracold molecules represent a powerful platform for quantum science due to their rich and controllable internal degrees of freedom. However, the detection of correlations between single molecules in an ultracold gas has yet to be demonstrated. Here we observe the Hanbury Brown and Twiss effect in a gas of bosonic $^{23}$Na$^{87}$Rb, enabled by the realization of a quantum gas microscope for molecules. We detect the characteristic bunching correlations in the densit…
We propose an experimentally realizable scheme to produce triatomic ultralong-range Rydberg molecules (TURM), formed in ultracold KRb traps. A near resonant coupling of the non-zero quantum defect Rydberg levels with the KRb molecule in N=0 and N=2 rotational levels, is engineered which exploits the unique Rydberg electron-molecule anisotropic dipole interaction. This near resonant coupling enhances the TURM binding and produces favorable Franck-Condon factors. Schemes for both postassium and rubidium excitations are demonstrated.
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 that laser excitations can coherently induce a novel Kondo effect in ultracold atoms in optical lattices. Using a model of alkaline-earth fermions with two orbitals, it is shown that the optically coupled two internal states are dynamically entangled to form the Kondo-singlet state, overcoming the heating effect due to the irradiation. Furthermore, a lack of SU($N$) symmetry in the optical coupling provides a peculiar feature in the Kondo effect, which results in spin-selective renormalization of effective masses. We also discuss effects of interorbital exchange interactions, an…
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 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 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 spectral properties of a finite laser-driven lattice of ultracold Rydberg atoms exploiting the dipole blockade effect in the frozen Rydberg gas regime. Uniform one-dimensional lattices as well as lattices with variable spacings are considered. In the case of a weak laser coupling, we find a multitude of many-body Rydberg states with well-defined excitation properties which are adiabatically accessible starting from the ground state. A comprehensive analysis of the degeneracies of the spectrum as well as of the single and pair excitations numbers of the eigenstates is perform…
We report on the creation of ultracold 84Sr2 molecules in the electronic ground state. The molecules are formed from atom pairs on sites of an optical lattice using stimulated Raman adiabatic passage (STIRAP). We achieve a transfer efficiency of 30% and obtain 4x10^4 molecules with full control over the external and internal quantum state. STIRAP is performed near the narrow 1S0-3P1 intercombination transition, using a vibrational level of the 0u potential as intermediate state. In preparation of our molecule association scheme, we have determined the binding energies of the last vibrational l…
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 …
The lifetime of nonreactive ultracold bialkali gases was conjectured to be limited by sticky collisions amplifying three-body loss. We show that the sticking times were previously overestimated and do not support this hypothesis. We find that electronic excitation of NaK+NaK collision complexes by the trapping laser leads to the experimentally observed two-body loss. We calculate the excitation rate with a quasiclassical, statistical model employing ab initio potentials and transition dipole moments. Using longer laser wavelengths or repulsive box potentials may suppress the losses.
For two states of opposite parity that cross as a function of an external magnetic field, the addition of an electric field will break the symmetry and induce an avoided crossing. A suitable arrangement of fields may be used to create a conical intersection as a function of external spatial coordinates. We consider the effect of the resulting geometric phase for ultracold polar molecules. For a Bose-Einstein condensate in the mean-field approximation, the geometric phase effect induces stable states of persistent superfluid flow that are characterized by half-integer quantized angular momentum…
We produce ultracold dense trapped samples of 87Rb133Cs molecules in their rovibrational ground state, with full nuclear hyperfine state control, by stimulated Raman adiabatic passage (STIRAP) with efficiencies of 90%. We observe the onset of hyperfine-changing collisions when the magnetic field is ramped so that the molecules are no longer in the hyperfine ground state. A strong quadratic shift of the transition frequencies as a function of applied electric field shows the strongly dipolar character of the RbCs ground-state molecule. Our results open up the prospect of realizing stable bosoni…
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 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.
We report on the creation of bosonic NaCs molecules in their absolute rovibrational ground state via stimulated Raman adiabatic passage. We create ultracold gases with up to 22,000 dipolar NaCs molecules at a temperature of 300(50) nK and a peak density of $1.0(4) \times 10^{12}$ cm$^{-3}$. We demonstrate comprehensive quantum state control by preparing the molecules in a specific electronic, vibrational, rotational, and hyperfine state. Employing the tunability and strength of the permanent electric dipole moment of NaCs, we induce dipole moments of up to 2.6 D. Dipolar systems of NaCs molecu…
