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In the quest toward realizing novel quantum matter in ultracold molecular gases, we perform a numerical study of evaporative cooling in ultracold gases of microwave-shielded polar fermionic molecules. Our Monte Carlo simulations incorporate accurate two-body elastic and inelastic scattering cross sections, realistic modeling of the optical dipole trap, and the influence of Pauli blocking at low temperatures. The simulations are benchmarked against data from evaporation studies performed with ultracold NaK molecules, showing excellent agreement. We further explore the prospects for optimizing the evaporation efficiency by varying the ramp rate and duration of the evaporation trajectory. Our simulation shows that it is possible to reach $< 10\%$ of the Fermi temperature under optimal conditions even in the presence of two-body molecular losses., Comment: 12 pages, 9 figures, 2 tables

We present a deperturbation analysis of the spin-orbit coupled $\rm A^1\Sigma^+$ and $\rm b^3\Pi_{0^+}$ states of LiRb based on the rovibrational energy levels observed previously by photoassociation spectroscopy in bosonic $^7$Li$^{85}$Rb molecule. Using the genetic algorithm, we fit the potential energy curves of the $\rm A^1\Sigma^+$ state and the $\rm b^3\Pi$ state into point-wise form. We then fit these point-wise potentials along with the spin-orbit coupling into expanded Morse oscillator functional form and optimise analytical parameters based on the experimental data. From the fitted results, we calculate the transition dipole moment matrix elements for transitions from the rovibrational levels of the coupled $\rm A^1\Sigma^+$-$\rm b^3\Pi_{0^+}$ state to the Feshbach state and the absolute rovibrational ground state for fermionic $^6$Li$^{87}$Rb molecule. Based on the calculated transition dipole moment matrix elements, several levels of the coupled $\rm A^1\Sigma^+$-$\rm b^3\Pi_{0^+}$ state are predicted to be suitable as the intermediate state for stimulated Raman adiabatic passage transfer from the Feshbach state to the absolute rovibrational ground state. In addition, we also provide a similar estimation for ${\rm B}^1\Pi$-${\rm c}^3\Sigma_1^+$-${\rm b}^3\Pi_1$ state based on available $ab\ initio$ interaction potentials., Comment: 12 pages, 9 figures

We investigate the static and dynamic properties of tetratomic molecules formed by two microwave-shielded polar molecules across field-linked resonances. In particular, we focus on two-body physics and experimental techniques unexplored in the recent experiment [X.-Y. Chen {\it et al}., Nature {\bf626}, 283 (2024)]. We show that, compared to the lowest tetramer state, higher tetramer states typically have longer lifetimes, which may facilitate a further cooling of tetramer gases towards quantum degeneracy. To detect tetramers, we identify the distinctive time-of-flight images from ramp dissociation, which can be observed by lowering the ramp rate of the microwave. Remarkably, in the modulational dissociation of tetramers, we find that multi-photon processes induce dissociation even below the threshold modulation frequency when the modulation amplitude is sufficiently high. Given the universal form of the inter-molecular potential for microwave-shielded polar molecules, our results also apply to other molecular gases widely explored in recent experiments.

Ultracold polyatomic molecules offer intriguing new opportunities in cold chemistry, precision measurements, and quantum information processing, thanks to their rich internal structure. However, their increased complexity compared to diatomic molecules presents a formidable challenge to employ conventional cooling techniques. Here, we demonstrate a new approach to create ultracold polyatomic molecules by electroassociation in a degenerate Fermi gas of microwave-dressed polar molecules through a field-linked resonance. Starting from ground state NaK molecules, we create around $1.1\times 10^3$ tetratomic (NaK)$_2$ molecules, with a phase space density of $0.040(3)$ at a temperature of $134(3)\,\text{nK}$, more than $3000$ times colder than previously realized tetratomic molecules. We observe a maximum tetramer lifetime of $8(2)\,\text{ms}$ in free space without a notable change in the presence of an optical dipole trap, indicating these tetramers are collisionally stable. The measured binding energy and lifetime agree well with parameter-free calculations, which outlines pathways to further increase the lifetime of the tetramers. Moreover, we directly image the dissociated tetramers through microwave-field modulation to probe the anisotropy of their wave function in momentum space. Our result demonstrates a universal tool for assembling ultracold polyatomic molecules from smaller polar molecules, which is a crucial step towards Bose--Einstein condensation (BEC) of polyatomic molecules and towards a new crossover from a dipolar Bardeen-Cooper-Schrieffer (BCS) superfluid to a BEC of tetramers. Additionally, the long-lived FL state provides an ideal starting point for deterministic optical transfer to deeply bound tetramer states.

The formation of bulk metallic glass requires the constituent elements to have a negative heat of mixing but has no restrictions on its magnitude. An understanding of this issue is lacking due to the absence of a valid method for describing chemical ordering of metallic glasses. For example, the radial distribution function is ineffective in identifying the elemental preferences of packed atoms. Here, we show that using molecular-dynamics simulation, the chemical medium-range ordering of liquid alloys can be evaluated from persistent homology. This inherently arising chemical medium-range order in metallic glasses is exclusively regulated by the activation and inhibition of the constituent components, making the topology of metallic glasses a Turing pattern. The connecting schemes of atoms of the same species form three distinct regions, reflecting different correlations at the short and medium length scales, while the difference in the schemes corresponds to chemical ordering. By changing the elemental types, it is demonstrated that the chemical medium-range order strongly depends on the relative depth of the interatomic-potential wells. The study separates metallic glasses from crystals under the condition of negative heat of mixing by emphasizing their fundamental difference in interatomic potentials.

Collisional complexes, which are formed as intermediate states in molecular collisions, are typically short-lived and decay within picoseconds. However, in ultracold collisions involving bialkali molecules, complexes can live for milliseconds, completely changing the collision dynamics. This can lead to unexpected two-body loss in samples of nonreactive molecules. During the last decade, such "sticky" collisons have been a major hindrance in the preparation of dense and stable molecular samples, especially in the quantum-degenerate regime. Currently, the behavior of the complexes is not fully understood. For example, in some cases their lifetime has been measured to be many orders of magnitude longer than recent models predict. This is not only an intriguing problem in itself but also practically relevant, since understanding molecular complexes may help to mitigate their detrimental effects. Here, we review the recent experimental and theoretical progress in this field. We treat the case of molecule-molecule as well as molecule-atom collisions., Comment: 15 pages, 7 figures. Comments and suggestions welcome

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 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 superfluids and molecular supersolids as well as assembling ultracold polyatomic molecules.

For microwave-dressed polar molecules, we analytically derive an intermolecular potential composed of an anisotropic van der Waals shielding core and a long-range dipolar interaction. We validate this effective potential by comparing its scattering properties with those calculated using the full multi-channel interaction potential. It is shown that scattering resonances can be induced by a sufficiently strong microwave field. We also show the power of the effective potential in the study of many-body physics by calculating the critical temperature of the Bardeen-Cooper-Schrieffer pairing in the microwave-dressed NaK gas. It turns out that the effective potential is well-behaved and extremely suitable for studying the many-body physics of the molecular gases. Our results pave the way for the studies of the many-body physics of the ultracold microwave-dressed molecular gases.

Ultracold fermionic Feshbach molecules are promising candidates for exploring quantum matter with strong $p$-wave interactions, however, their lifetimes were measured to be short. Here, we characterize the $p$-wave collisions of ultracold fermionic $^{23}\mathrm{Na}^{40}\mathrm{K}$ Feshbach molecules for different scattering lengths and temperatures. By increasing the binding energy of the molecules, the two-body loss coefficient reduces by three orders of magnitude leading to a second-long lifetime, 20 times longer than that of ground-state molecules. We exploit the scaling of elastic and inelastic collisions with the scattering length and temperature to identify a regime where the elastic collisions dominate over the inelastic ones allowing the molecular sample to thermalize. Our work provides a benchmark for four-body calculations of molecular collisions and is essential for producing a degenerate Fermi gas of Feshbach molecules.

Ultracold polar molecules offer strong electric dipole moments and rich internal structure, which makes them ideal building blocks to explore exotic quantum matter, implement novel quantum information schemes, or test fundamental symmetries of nature. Realizing their full potential requires cooling interacting molecular gases deeply into the quantum degenerate regime. However, the complexity of molecules which makes their collisions intrinsically unstable at the short range, even for nonreactive molecules, has so far prevented the cooling 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 down to 21 nanokelvin, corresponding to 0.36 times the Fermi temperature. Such unprecedentedly cold and dense samples of polar molecules open the path to the exploration of novel many-body phenomena, such as the long-sought topological p-wave superfluid states of ultracold matter., Comment: 11 pages, 7 figures

The interplay of quantum statistics and interactions in atomic Bose--Fermi mixtures leads to a phase diagram markedly different from pure fermionic or bosonic systems. However, investigating this phase diagram remains challenging when bosons condense. Here, we observe evidence for a quantum phase transition from a polaronic to a molecular phase in a density-matched degenerate Bose--Fermi mixture. The condensate fraction, representing the order parameter of the transition, is depleted by interactions and the build-up of strong correlations results in the emergence of a molecular Fermi gas. By driving through the transition, we ultimately produce a quantum-degenerate sample of sodium-potassium molecules exhibiting a large molecule-frame dipole moment of 2.7 Debye. The observed phase transition represents a new phenomenon complementary to the paradigmatic BEC-BCS crossover observed in Fermi systems., Comment: 12 pages, 9 figures

We study three-body loss in an ultracold mixture of a thermal Bose gas and a degenerate Fermi gas. We find that at unitarity, where the interspecies scattering length diverges, the usual inverse-square temperature scaling of the three-body loss found in non-degenerate systems is strongly modified and reduced with the increasing degeneracy of the Fermi gas. While the reduction of loss is qualitatively explained within the few-body scattering framework, a remaining suppression provides evidence for the long-range RKKY interactions mediated by fermions between bosons. Our model based on RKKY interactions quantitatively reproduces the data without free parameters, and predicts one order of magnitude reduction of the three-body loss coefficient in the deeply Fermi-degenerate regime.

We demonstrate the transfer of $^{23}$Na$^{40}$K molecules from a closed-channel dominated Feshbach-molecule state to the absolute ground state. The Feshbach molecules are initially created from a gas of sodium and potassium atoms via adiabatic ramping over a Feshbach resonance at 78.3$\,$G. The molecules are then transferred to the absolute ground state using stimulated Raman adiabatic passage with an intermediate state in the spin-orbit-coupled complex $|c^3 \Sigma^+, v=35, J=1 \rangle \sim |B^1\Pi, v=12, J=1\rangle$. Our measurements show that the pump transition dipole moment linearly increases with the closed-channel fraction. Thus, the pump-beam intensity can be two orders of magnitude lower than is necessary with open-channel dominated Feshbach molecules. We also demonstrate that the phase noise of the Raman lasers can be reduced by filter cavities, significantly improving the transfer efficiency., Comment: 8 pages, 7 figures

Understanding collisions between ultracold molecules is crucial for making stable molecular quantum gases and harnessing their rich internal degrees of freedom for quantum engineering. Transient complexes can strongly influence collisional physics, but in the ultracold regime, key aspects of their behavior have remained unknown. To explain experimentally observed loss of ground-state molecules from optical dipole traps, it was recently proposed that molecular complexes can be lost due to photo-excitation. By trapping molecules in a repulsive box potential using laser light near a narrow molecular transition, we are able to test this hypothesis with light intensities three orders of magnitude lower than what is typical in red-detuned dipole traps. This allows us to investigate light-induced collisional loss in a gas of nonreactive fermionic $^{23}$Na$^{40}$K molecules. Even for the lowest intensities available in our experiment, our results are consistent with universal loss, meaning unit loss probability inside the short-range interaction potential. Our findings disagree by at least two orders of magnitude with latest theoretical predictions, showing that crucial aspects of molecular collisions are not yet understood, and provide a benchmark for the development of new theories., Comment: 13 pages, 11 figures

We demonstrate a versatile, rotational-state dependent trapping scheme for the ground and first excited rotational states of $^{23}$Na$^{40}$K molecules. Close to the rotational manifold of a narrow electronic transition, we determine tune-out frequencies where the polarizability of one state vanishes while the other remains finite, and a magic frequency where both states experience equal polarizability. The proximity of these frequencies of only 10 GHz allows for dynamic switching between different trap configurations in a single experiment, while still maintaining sufficiently low scattering rates., Comment: 11 pages, 10 figures

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 bulk gas., Comment: 10 pages, 8 figures

Interferometry is a paradigm for most precision measurements. Using $N$ uncorrelated particles, the achievable precision for a two-mode (two-path) interferometer is bounded by the standard quantum limit (SQL), $1/\sqrt{N}$, due to the discrete (quanta) nature of individual measurements. Despite being a challenging benchmark, the two-mode SQL has been approached in a number of systems, including the LIGO and today's best atomic clocks. Employing multi-mode interferometry, the SQL becomes $1/[(M-1)\sqrt{N}]$ using M modes. Higher precision can also be achieved using entangled particles such that quantum noises from individual particles cancel out. In this work, we demonstrate an interferometric precision of $2.42^{+1.76}_{-1.29}\,$dB beyond the three-mode SQL, using balanced spin-1 (three-mode) Dicke states containing thousands of entangled atoms. The input quantum states are deterministically generated by controlled quantum phase transition and exhibit close to ideal quality. Our work shines light on the pursuit of quantum metrology beyond SQL., Comment: 11 pages, 6 figures

In this work we model and realize stimulated Raman adiabatic passage (STIRAP) in the diatomic $\mathrm{^{23}Na^{40}K}$ molecule from weakly bound Feshbach molecules to the rovibronic ground state via the $\left|v_d=5,J=\Omega=1\right\rangle$ excited state in the $d^3\Pi$ electronic potential. We demonstrate how to set up a quantitative model for polar molecule production by taking into account the rich internal structure of the molecules and the coupling laser phase noise. We find excellent agreement between the model predictions and the experiment, demonstrating the applicability of the model in the search of an ideal STIRAP transfer path. In total we produce 5000 fermionic groundstate molecules. The typical phase-space density of the sample is 0.03 and induced dipole moments of up to 0.54 Debye could be observed., Comment: 7 pages, 5 figures Version 2: Fixed a few typos, elaborated more on the differences between different choices of intermediate state, clarified H\"onl-London factor, added a intuitive explanation of the benefits of detuned STIRAP, elaborated on realized dipole moments in diatomics, compared phase-space density reducing processes in the whole molecule creation process, added two more references

Many-body entanglement is often created through system evolution, aided by non-linear interactions between the constituting particles. The very dynamics, however, can also lead to fluctuations and degradation of the entanglement if the interactions cannot be controlled. Here, we demonstrate near-deterministic generation of an entangled twin-Fock condensate of $\sim11000$ atoms by driving a $^{87}$Rb Bose-Einstein condensate undergoing spin mixing through two consecutive quantum phase transitions (QPTs). We directly observe number squeezing of $10.7\pm0.6$ dB and normalized collective spin length of $0.99\pm0.01$. Together, these observations allow us to infer an entanglement-enhanced phase sensitivity of $\sim6$ dB beyond the standard quantum limit and an entanglement breadth of $\sim910$ atoms. Our work highlights the power of generating large-scale useful entanglement by taking advantage of the different entanglement landscapes separated by QPTs., Comment: Supplementary materials can be found at http://science.sciencemag.org/content/355/6325/620/tab-figures-data

Spin-orbit coupling (SOC) plays an essential role in many exotic and interesting phenomena in condensed matter physics. In neutral-atom-based quantum simulations, synthetic SOC constitutes a key enabling element. The strength of SOC realized so far is limited by various reasons or constraints. This work reports tunable SOC synthesized with a gradient magnetic field (GMF) for atoms in a harmonic trap. Nearly ten-fold enhancement is observed when the GMF is modulated near the harmonic-trap resonance in comparison with free-space atoms. A theory is developed that well explains the experimental results. Our work offers a clear physical insight into and analytical understanding of how to tune the strength of atomic SOC synthesized with GMF using harmonic trap resonance., Comment: 5 pages, 1 figure