Quantum states with long-lived coherence are essential for quantum computation, simulation and metrology. The nuclear spin states of ultracold molecules prepared in the singlet rovibrational ground state are an excellent candidate for encoding and storing quantum information. However, it is important to understand all sources of decoherence for these qubits, and then eliminate them, in order to reach the longest possible coherence times. Here, we fully characterise the dominant mechanisms for decoherence of a storage qubit in an optically trapped ultracold gas of RbCs molecules using high-resolution Ramsey spectroscopy. Guided by a detailed understanding of the hyperfine structure of the molecule, we tune the magnetic field to where a pair of hyperfine states have the same magnetic moment. These states form a qubit, which is insensitive to variations in magnetic field. Our experiments reveal an unexpected differential tensor light shift between the states, caused by weak mixing of rotational states. We demonstrate how this light shift can be eliminated by setting the angle between the linearly polarised trap light and the applied magnetic field to a magic angle of $\arccos{(1/\sqrt{3})}\approx55^{\circ}$. This leads to a coherence time exceeding 6.9 s (90% confidence level). Our results unlock the potential of ultracold molecules as a platform for quantum computation.
High-density and ultracold atomic gases have emerged as promising media for storage of individual photons for quantum memory applications. In this paper we provide an overview of our theoretical and experimental efforts in this direction, with particular attention paid to manipulation of light storage (a) through complex recurrent optical scattering processes in very high density gases (b) by an external control field in a characteristic electromagnetically induced transparency configuration.
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 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 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 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 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 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…
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.
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 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 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 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…
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…
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…
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）
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,…
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 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…
Ultracold high-spin $Σ$-state polar molecules for new physics searches
Istituto Nazionale di Ottica del Consiglio Nazionale delle Ricerche (CNR-INO)（意大利国家光学研究所）；European Laboratory for Non-Linear Spectroscopy (LENS), Università di Firenze（欧洲非线性光谱学实验室，佛罗伦萨大学）；Faculty of Physics, University of Warsaw（华沙大学物理学院）
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…
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{…
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 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 explore the dynamical transport of an impurity between different embedding majority species which are spatially separated in a double well. The transfer and storage of the impurity is triggered by dynamically changing the interaction strengths between the impurity and the two majority species. We find a simple but efficient protocol consisting of linear ramps of majority-impurity interactions at designated times to pin or unpin the impurity. Our study of this highly imbalanced few-body triple mixture is conducted with the multi-layer multi-configuration time-dependent Hartree method for ato…
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.
We show how to use polar molecules in an optical lattice to engineer quantum spin models with arbitrary spin S >= 1/2 and with interactions featuring a direction-dependent spin anisotropy. This is achieved by encoding the effective spin degrees of freedom in microwave-dressed rotational states of the molecules and by coupling the spins through dipolar interactions. We demonstrate how one of the experimentally most accessible anisotropies stabilizes symmetry protected topological phases in spin ladders. Using the numerically exact density matrix renormalization group method, we find that these …
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.
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…
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…
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$^{-2}$.
We design dipolar quantum many-body Hamiltonians that will facilitate the realization of exotic quantum phases under current experimental conditions achieved for polar molecules. The main idea is to modulate both single-body potential barriers and two-body dipolar interactions on a spatial scale of tens of nanometers to strongly enhance energy scales and, therefore, relax temperature requirements for observing new quantum phases of engineered many-body systems. We consider and compare two approaches. In the first, nanoscale barriers are generated with standing wave optical light fields exploit…
In this article we address the general approach for calculating dynamical dipole polarizabilities of small quantum systems, based on a sum-over-states formula involving in principle the entire energy spectrum of the system. We complement this method by a few-parameter model involving a limited number of effective transitions, allowing for a compact and accurate representation of both the isotropic and anisotropic components of the polarizability. We apply the method to the series of ten heteronuclear molecules composed of two of ($^7$Li,$^{23}$Na,$^{39}$K,$^{87}$Rb,$^{133}$Cs) alkali-metal ato…
We study the checkerboard supersolid of the hard-core Bose-Hubbard model with the dipole-dipole interaction. This supersolid is different from all other supersolids found in lattice models in the sense that superflow paths through which interstitials or vacancies can hop freely are absent in the crystal. By focusing on repulsive interactions between interstitials, we reveal that the long-range tail of the dipole-dipole interaction have the role of increasing the energy cost of domain wall formations. This effect produces the supersolid by the second-order hopping process of defects. We also pe…
Generation of strong ultralow-phase-noise microwave fields with tunable ellipticity for ultracold polar molecules
Max-Planck-Institut für Quantenoptik（马克斯·普朗克量子光学研究所）；Munich Center for Quantum Science and Technology（慕尼黑量子科学与技术中心）；Technische Universität München（慕尼黑工业大学）；Vienna Center for Quantum Science and Technology, Atominstitut, TU Wien（维也纳量子科学与技术中心，原子研究所，维也纳工业大学）；Fakultät für Physik, Ludwig-Maximilians-Universität（路德维希-马克西米利安大学物理学院）
The notion of a polaron, originally introduced in the context of electrons in ionic lattices, helps us to understand how a quantum impurity behaves when being immersed in and interacting with a many-body background. We discuss the impact of the impurities on the medium particles by considering feedback effects from polarons that can be realized in ultracold quantum gas experiments. In particular, we exemplify the modifications of the medium in the presence of either Fermi or Bose polarons. Regarding Fermi polarons we present a corresponding many-body diagrammatic approach operating at finite t…
We analyze the dynamics of Bose polarons in the vicinity of a Feshbach resonance between the impurity and host atoms. We compute the radio-frequency absorption spectra for the case when the initial state of the impurity is non-interacting and the final state is strongly interacting. We compare results of different theoretical approaches including a single excitation expansion, a self-consistent T-matrix method, and a time-dependent coherent state approach. Our analysis reveals sharp spectral features arising from metastable states with several Bogoliubov excitations bound to the impurity atom.…
Polaron quasiparticles are formed when a mobile impurity is coupled to the elementary excitations of a many-particle background. In the field of ultracold atoms, the study of the associated impurity problem has attracted a growing interest over the last fifteen years. Polaron quasiparticle properties are essential to our understanding of a variety of paradigmatic quantum many-body systems realized in ultracold atomic gases and in the solid state, from imbalanced Bose-Fermi and Fermi-Fermi mixtures to fermionic Hubbard models. In this topical review, we focus on the so-called repulsive polaron …
We present a quantitative, near-term experimental blueprint for the quantum simulation of topological insulators using lattice-trapped ultracold polar molecules. In particular, we focus on the so-called Hopf insulator, which represents a three-dimensional topological state of matter existing outside the conventional tenfold way and crystalline-symmetry-based classifications of topological insulators. Its topology is protected by a \emph{linking number} invariant, which necessitates long-range spin-orbit coupled hoppings for its realization. While these ingredients have so far precluded its rea…
The field of ultracold quantum matter has burgeoned over the last few decades, thanks to the growing capabilities for atomic systems to be probed and manipulated with exquisite control. Researchers can now precisely create and study quantum many-body states that are effectively isolated from the external environment. Much of the work in ultracold matter has focused on systems of alkali or alkaline-earth atoms, mainly due to their ease of cooling. Extending this precise control to molecules has seen rapidly increasing interest and activity, as molecules possess additional degrees of freedom tha…
