Ultracold Polar Molecules Research Articles

Magnetically Tunable Electric Dipolar Interactions of Ultracold Polar Molecules in the Quantum Ergodic Regime.

By leveraging the hyperfine interaction between the rotational and nuclear spin degrees of freedom, we demonstrate extensive magnetic control over the electric dipole moments, electric dipolar interactions, and ac Stark shifts of ground-state alkali-dimer molecules such as KRb(X^{1}Σ^{+}). The control is enabled by narrow avoided crossings and the highly ergodic character of molecular eigenstates at low magnetic fields, offering a general and robust way of continuously tuning the intermolecular electric dipolar interaction for applications in quantum simulation, quantum sensing, and dipolar spinor physics.

Quantum sensing of ultralow temperature in biwire ultracold polar molecules

Quantum sensing of ultralow temperature in biwire ultracold polar molecules

Quantum gate control of polar molecules with machine learning.

We propose a scheme for achieving basic quantum gates using ultracold polar molecules in pendular states. The qubits are encoded in the YbF molecules trapped in an electric field with a certain gradient and coupled by the dipole-dipole interaction. The time-dependent control sequences consisting of multiple pulses are considered to interact with the pendular qubits. To achieve high-fidelity quantum gates, we map the control problem for the coupled molecular system into a Markov decision process and deal with it using the techniques of deep reinforcement learning (DRL). By training the agents over multiple episodes, the optimal control pulse sequences for the two-qubit gates of NOT, controlled NOT, and Hadamard are discovered with high fidelities. Moreover, the population dynamics of YbF molecules driven by the discovered gate sequences are analyzed in detail. Furthermore, by combining the optimal gate sequences, we successfully simulate the quantum circuit for entanglement. Our findings could offer new insights into efficiently controlling molecular systems for practical molecule-based quantum computing using DRL.

Raman Sideband Cooling of Molecules in an Optical Tweezer Array to the 3D Motional Ground State

Ultracold polar molecules are promising for quantum information processing and searches for physics beyond the standard model. Laser cooling to ultracold temperatures is an established technique for trapped diatomic and triatomic molecules. Further cooling of the molecules to near the motional ground state is crucial for reducing various dephasings in quantum and precision applications. In this work, we demonstrate Raman sideband cooling (RSC) of CaF molecules in optical tweezers to near their motional ground state, with average motional occupation quantum numbers of n¯x=0.16(12), n¯y=0.17(17) (radial directions), and n¯z=0.22(16) (axial direction), and a 3-D motional-ground-state probability of 54±18% of the molecules that survive the RSC. This process paves the way to increase molecular coherence times in optical tweezers for robust quantum computation and simulation applications. Published by the American Physical Society 2024

Ultracold LiCr : A New Pathway to Quantum Gases of Paramagnetic Polar Molecules

Quantum gases of doubly polar molecules represent appealing frameworks for a variety of cross-disciplinary applications, encompassing quantum simulation and computation, controlled quantum chemistry, and precision measurements. Through a joint experimental and theoretical study, here we explore a novel class of ultracold paramagnetic polar molecules combining lithium alkali and chromium transition metal elements. Focusing on the specific bosonic isotopologue 6Li53Cr, leveraging on the Fermi statistics of the parent atomic mixture and on suitable Feshbach resonances recently discovered, we produce up to 50×103 ultracold LiCr molecules at peak phase-space densities exceeding 0.1, prepared within the least bound rotationless level of the LiCr electronic ground state X6Σ+. By also developing new probing methods, we thoroughly characterize the molecular gas, demonstrating the paramagnetic nature of LiCr dimers and the precise control of their quantum state. We investigate their stability against inelastic processes and identify a parameter region where pure LiCr samples exhibit lifetimes exceeding 0.2 s. Parallel to this, we employ state-of-the-art quantum chemical calculations to accurately predict the properties of LiCr ground and excited electronic states. This model, able to reproduce the experimental Li-Cr high-spin, scattering length, allows us to identify both efficient paths to coherently transfer weakly bound LiCr dimers to their absolute ground state, and suitable transitions for their subsequent optical manipulation. Our studies establish Li-Cr as a prime candidate to realize ultracold gases of doubly polar molecules with significant electric (3.3 D) and magnetic (5μB) dipole moments. Published by the American Physical Society 2024

Fine Control of Ultracold Polar Molecules

Fine Control of Ultracold Polar Molecules

Second-scale rotational coherence and dipolar interactions in a gas of ultracold polar molecules

Ultracold polar molecules combine a rich structure of long-lived internal states with access to controllable long-range anisotropic dipole–dipole interactions. In particular, the rotational states of polar molecules confined in optical tweezers or optical lattices may be used to encode interacting qubits for quantum computation or pseudo-spins for simulating quantum magnetism. As with all quantum platforms, the engineering of robust coherent superpositions of states is vital. However, for optically trapped molecules, the coherence time between rotational states is typically limited by inhomogeneous differential light shifts. Here we demonstrate a rotationally magic optical trap for 87Rb133Cs molecules that supports a Ramsey coherence time of 0.78(4) s in the absence of dipole–dipole interactions. This is estimated to extend to >1.4 s at the 95% confidence level using a single spin-echo pulse. In our trap, dipolar interactions become the dominant mechanism by which Ramsey contrast is lost for superpositions that generate oscillating dipoles. By changing the states forming the superposition, we tune the effective dipole moment and show that the coherence time is inversely proportional to the strength of the dipolar interaction. Our work unlocks the full potential of the rotational degree of freedom in molecules for quantum computation and quantum simulation.

Implementation of three-qubit Deutsch-Jozsa algorithm with pendular states of polar molecules by optimal control

Ultracold polar molecules have gained much attention as a potential candidate for quantum information processing due to their long coherence time and strong dipole–dipole interaction. In the present study, we explore the dynamics of three polar molecules that are mutually coupled and arranged in an equilateral triangle configuration within a gradient electric field. By employing the pendular states of polar molecules as qubits, we simulate the three-qubit Deutsch-Jozsa algorithm via multi-target optimal control. Through the design of optimal microwave pulses with multiple iterations, our approach can accomplish the operations required to complete the algorithm in a single operational step with high fidelity and large transition probability. Furthermore, we compare and analyze the fidelity and average transition probability with respect to iteration numbers for each unitary operation Uf pulse. It is found that by combining the optimized X, H⊗H⊗H, Uf, and H⊗H gate pulses, the Deutsch-Jozsa algorithm in the three-dipole system can be performed well for distinguishing between constant and balanced functions. Our findings could shed some light on the physical realization of multi-particle quantum algorithm based on polar molecules in external electric fields.

Alignment transport between ultracold polar molecules.

We propose an array of ultracold polar molecules as a platform to study alignment transport between molecules. We envision a polar molecule being aligned with an intense off-resonant laser field whose alignment migrates to a nearby molecule due to dipole-dipole interactions. Our results show that the transport of the alignment is due to a complex interplay between electric field-driven excitations and dipole-dipole interactions. All mechanisms for alignment transfer are elucidated and analyzed. Using NaCs as a prototype molecule, we find that the time for alignment transfer is (10 μs), which makes the phenomena readily observable in the lab.

Dipolar spin-exchange and entanglement between molecules in an optical tweezer array

Ultracold polar molecules are promising candidate qubits for quantum computing and quantum simulations. Their long-lived molecular rotational states form robust qubits, and the long-range dipolar interaction between molecules provides quantum entanglement. In this work, we demonstrate dipolar spin-exchange interactions between single calcium monofluoride (CaF) molecules trapped in an optical tweezer array. We realized the spin- 1 2 quantum XY model by encoding an effective spin- 1 2 system into the rotational states of the molecules and used it to generate a Bell state through an iSWAP operation. Conditioned on the verified existence of molecules in both tweezers at the end of the measurement, we obtained a Bell state fidelity of 0.89(6). Using interleaved tweezer arrays, we demonstrate single-site molecular addressability.

A new route to associating ultracold polar molecules in the absolute ground state

A new route to associating ultracold polar molecules in the absolute ground state

Efficient production of ultracold polar molecules 23Na40K in their absolute ground state via intermediate state of the coupled complex B1Π|ν = 4〉 ∼ c3Σ+ |ν = 25〉

Efficient production of ultracold polar molecules 23Na40K in their absolute ground state via intermediate state of the coupled complex B1Π|ν = 4〉 ∼ c3Σ+ |ν = 25〉

Two-photon optical shielding of collisions between ultracold polar molecules

Two-photon optical shielding of collisions between ultracold polar molecules

Operator growth from global out-of-time-order correlators

In chaotic many-body systems, scrambling or the operator growth can be diagnosed by out-of-time-order correlators of local operators. We show that operator growth also has a sharp imprint in out-of-time-order correlators of global operators. In particular, the characteristic spacetime shape of growing local operators can be accessed using global measurements without any local control or readout. Building on an earlier conjectured phase diagram for operator growth in chaotic systems with power-law interactions, we show that existing nuclear spin data for out-of-time-order correlators of global operators are well fit by our theory. We also predict super-polynomial operator growth in dipolar systems in 3d and discuss the potential observation of this physics in future experiments with nuclear spins and ultra-cold polar molecules.

Simulation of Grover Search with Polar CH3CN Molecules by Optimal Control Fields

AbstractTheoretical schemes for the implementation of the Grover search algorithm are proposed based on ultracold polar molecules in an electric field. The molecular qubits and qudit are chosen as the field‐dressed states formed by the rotational modes of CH3CN. With the help of multi‐target optimal control theory, the microwave pulses for the elementary logic operations including the one‐qubit Hadamard gates and the conditional phase gates in a dipole‐dipole system are designed and the factorized Grover algorithm demonstrated using two coupled CH3CN molecules. To reduce the accumulation of imprecision and decoherence resulting from the combination of multiple elementary gates, the optimal pulses that can achieve the two‐qubit Hadamard gate and diffusion operation in one step are designed successfully. In this way, the probabilities to find the states corresponding to the desired elements in an unsorted database are enhanced to some extent. Moreover, the optimal pulse sequence suitable for a four‐level molecular qudit, which can be used to simulate the quantum search on a single CH3CN molecule with high fidelity, is designed. These results can shed some light on the physical realization of quantum computing based on ultracold polyatomic molecules.

Field-linked resonances of polar molecules

Scattering resonances are an essential tool for controlling the interactions of ultracold atoms and molecules. However, conventional Feshbach scattering resonances1, which have been extensively studied in various platforms1–7, are not expected to exist in most ultracold polar molecules because of the fast loss that occurs when two molecules approach at a close distance8–10. Here we demonstrate a new type of scattering resonance that is universal for a wide range of polar molecules. The so-called field-linked resonances11–14 occur in the scattering of microwave-dressed molecules because of stable macroscopic tetramer states in the intermolecular potential. We identify two resonances between ultracold ground-state sodium–potassium molecules and use the microwave frequencies and polarizations to tune the inelastic collision rate by three orders of magnitude, from the unitary limit to well below the universal regime. The field-linked resonance provides a tuning knob to independently control the elastic contact interaction and the dipole–dipole interaction, which we observe as a modification in the thermalization rate. Our result provides a general strategy for resonant scattering between ultracold polar molecules, which paves the way for realizing dipolar superfluids15 and molecular supersolids16, as well as assembling ultracold polyatomic molecules.

Probing site-resolved correlations in a spin system of ultracold molecules

Synthetic quantum systems with interacting constituents play an important role in quantum information processing and in explaining fundamental phenomena in many-body physics. Following impressive advances in cooling and trapping techniques, ensembles of ultracold polar molecules have emerged as a promising platform that combines several advantageous properties1-11. These include a large set of internal states with long coherence times12-17 and long-range, anisotropic interactions. These features could enable the exploration of intriguing phases of correlated quantum matter, such as topological superfluids18, quantum spin liquids19, fractional Chern insulators20 and quantum magnets21,22. Probing correlations in these phases is crucial to understanding their properties, necessitating the development of new experimental techniques. Here we use quantum gas microscopy23 to measure the site-resolved dynamics of quantum correlations of polar 23Na87Rb molecules confined in a two-dimensional optical lattice. By using two rotational states of the molecules, we realize a spin-1/2 system with dipolar interactions between particles, producing a quantum spin-exchange model21,22,24,25. We study the evolution of correlations during the thermalization process of an out-of-equilibrium spin system for both spatially isotropic and anisotropic interactions. Furthermore, we examine the correlation dynamics of a spin-anisotropic Heisenberg model engineered from the native spin-exchange model by using periodic microwave pulses26-28. These experiments push the frontier of probing and controlling interacting systems of ultracold molecules, with prospects for exploring new regimes of quantum matter and characterizing entangled states that are useful for quantum computation29,30 and metrology31.

Double-degenerate Fermi mixtures of Li6 and Cr53 atoms

We report on the realization of a novel degenerate mixture of ultracold fermionic lithium and chromium atoms. Based on an all-optical approach, with an overall duty-cycle of about 13 seconds, we produce large and degenerate samples of more than 2$\times 10^5$ $^6$Li atoms and $10^5$ $^{53}$Cr atoms, with both species exhibiting normalized temperatures of about $T/T_{F}$=0.25. Additionally, through the exploitation of a crossed bichromatic optical dipole trap, we can controllably vary the density and degree of degeneracy of the two components almost independently, and widely tune the lithium-to-chromium density ratio. Our $^{6}$Li-$^{53}$Cr Fermi mixture opens the way to the investigation of a variety of exotic few- and many-body regimes of quantum matter, and it appears as an optimally-suited system to realize ultracold paramagnetic polar molecules, characterized by both electric and magnetic dipole moments. Ultimately, our strategy also provides an efficient pathway to produce dipolar Fermi gases, or spin-mixtures, of ultracold $^{53}$Cr atoms.

Exploring Ultracold Collisions in ^{6}Li-^{53}Cr Fermi Mixtures: Feshbach Resonances and Scattering Properties of a Novel Alkali-Transition Metal System.

We investigate ultracold collisions in a novel mixture of ^{6}Li and ^{53}Cr fermionic atoms, discovering more than 50 interspecies Feshbach resonances via loss spectroscopy. Building a full coupled-channel model, we unambiguously characterize the ^{6}Li-^{53}Cr scattering properties and yield predictions for other isotopic pairs. In particular, we identify various Feshbach resonances that enable the controlled tuning of elastic s- and p-wave ^{6}Li-^{53}Cr interactions. Our studies thus make lithium-chromium mixtures emerge as optimally suited platforms for the experimental search of elusive few- and many-body regimes of highly correlated fermionic matter, and for the realization of a new class of ultracold polar molecules possessing both electric and magnetic dipole moments.

Evaporation of microwave-shielded polar molecules to quantum degeneracy

Ultracold polar molecules offer strong electric dipole moments and rich internal structure, which makes them ideal building blocks to explore exotic quantum matter1–9, implement quantum information schemes10–12 and test the fundamental symmetries of nature13. Realizing their full potential requires cooling interacting molecular gases deeply into the quantum-degenerate regime. However, the intrinsically unstable collisions between molecules at short range have so far prevented direct cooling through elastic collisions to quantum degeneracy in three dimensions. Here we demonstrate evaporative cooling of a three-dimensional gas of fermionic sodium–potassium molecules to well below the Fermi temperature using microwave shielding. The molecules are protected from reaching short range with a repulsive barrier engineered by coupling rotational states with a blue-detuned circularly polarized microwave. The microwave dressing induces strong tunable dipolar interactions between the molecules, leading to high elastic collision rates that can exceed the inelastic ones by at least a factor of 460. This large elastic-to-inelastic collision ratio allows us to cool the molecular gas to 21 nanokelvin, corresponding to 0.36 times the Fermi temperature. Such cold and dense samples of polar molecules open the path to the exploration of many-body phenomena with strong dipolar interactions.