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Andreas Schindewolf

Publications and source records attributed to Andreas Schindewolf.

At least 19 recordsLinked to original sources

Non-Additivity of Microwave-Shielded Interactions between Dipolar Molecules

Theoretical models of the effective interactions between microwave-shielded polar molecules typically rely on the assumption of pairwise additivity. In this work, we test the validity of this pairwise approximation by evaluating the exact many-body potential energy for configurations of three and four molecules. We demonstrate that this approximation fails for molecule configurations in the plane of the circularly polarized microwave field. In these planar geometries, many-body effects significantly increase the depth of the attractive potential well and shift the position of the repulsive barrier. Although out-of-plane interactions in three-dimensional arrangements weaken this non-additivity, the effective interactions between microwave-shielded dipoles are not a simple sum of pair interactions. In particular, their attractive well, crucial for self-bound clusters, can only be described by the full many-body potential energy.

cond-mat.quant-gas

A platform for nuclear symmetry-violation searches with laser-coolable molecules carrying spinful nuclei

Cold heavy molecules are promising systems for exploring nuclear $\mathcal{P}$- and $\mathcal{CP}$-violating phenomena in search of new physics beyond the Standard Model. However, most proposed experimental strategies and their early realizations to date have been limited to proof-of-principle molecular species with effectively spin-zero nuclei that are not sensitive to nuclear symmetry-violating phenomena. Here, we introduce a comprehensive experimental toolbox that integrates cooling, trapping, coherent state manipulation, and a complete precision-measurement protocol that is applicable to molecules carrying relevant nuclear spins. Using ${}^{137}$Ba${}^{19}$F and nuclear-spin-dependent parity violation (NSD-PV) as representative species and benchmark application, respectively, our approach achieves a projected statistical sensitivity roughly two orders of magnitude beyond comparable molecular beams by combining techniques already demonstrated individually in current experiments. This level of precision could provide realistic experimental access not only to the enhanced NSD-PV signals arising from the heavy ${}^{137}$Ba nucleus within this molecule but also to the contributions from the lighter ${}^{19}$F nucleus, bringing direct benchmarks of nuclear \textit{ab initio} theory within reach. We further identify a candidate magic wavelength as a route to second-scale rotational coherence in future experiments. The techniques developed here can be transferred to measurements of nuclear Schiff and magnetic quadrupole moments in molecules containing deformed nuclei, establishing a general platform for laboratory searches for nuclear symmetry violations.

physics.atom-ph

Engineering SU($N$)-Symmetric Hubbard Models with Microwave-Shielded Dipolar Molecules

Ultracold polar molecules provide strong, long-range interactions that microwave shielding makes tunable and nearly nuclear-spin independent, giving an emergent SU($N$) symmetry. However, extended Hubbard models of polar molecules in optical lattices lack, so far, controllable finite on-site interactions, a key ingredient of strong correlated physics. We show that tuning the Rabi frequency of the microwave coupling can bring two individual molecules (monomers) on neighboring lattice sites into resonance with a field-linked dimer (doublon) on one of the sites, enabling coherent doublon--monomer-pair conversion. In this model, we characterize the key Hubbard parameters and the dimer lifetime, demonstrating that the on-site and off-site interactions can be tuned nearly independently through the microwave amplitude and orientation, respectively. Our results provide a roadmap for implementing SU($N$)-symmetric extended Hubbard models with controllable doublon fluctuations, providing access to quantum-simulation in the strongly dipolar regime.

cond-mat.quant-gas

Equilibrium and non-equilibrium phases of microwave-dressed polar molecules beyond rotational symmetries

Recent experiments on molecular droplets have opened a new frontier of self-organization in strongly dipolar quantum matter. Microwave-dressing of polar molecules permits to tune both the strength and the angular structure of long-range interactions, potentially promoting a rich spectrum of quantum phases, from superfluid droplets with varying geometry and insulating or supersolid droplet arrays to strongly correlated crystals of individual molecules. Using path-integral Monte Carlo simulations of large molecular ensembles, we demonstrate that experimentally observed droplet arrays emerge as a metastable non-equilibrium state from the quenching of a gas-droplet phase transition under entirely broken rotational symmetry of the microwave-induced interaction potential. We moreover find that a crystalline phase of molecules, predicted for antidipolar interactions, is absent under conditions of recent experiments. This is traced back to the lack of angular symmetry in currently employed microwave-dressing, which qualitatively reshapes the many-body energy landscape and cannot be captured by effective scalar interaction parameters. Our results provide the first direct comparison of ab initio simulations and experiments and establish interaction anisotropy as a key aspect of molecular quantum gases.

cond-mat.quant-gas

Strongly dipolar molecular Bose-Einstein condensates: From few- to many-body physics

Recent advances in molecular cooling have enabled the realization of strongly dipolar Bose--Einstein condensates (BECs) of molecules, and BECs of many different molecular species may become experimentally accessible in the near future. Here, we explore the unique properties of such BECs and the new insights they may offer into dipolar quantum fluids and many-body physics. We explore which parameter regimes can realistically be achieved using currently available experimental techniques, discuss how to implement these techniques, and outline which molecular species are particularly well suited to explore exotic new states of matter. We further determine how state-of-the-art beyond mean-field theories, originally developed for weakly dipolar magnetic gases, can be pushed to their limits and beyond, and what other long-standing questions in the field of dipolar physics may realistically come within reach using molecular systems.

cond-mat.quant-gas

Generation of strong ultralow-phase-noise microwave fields with tunable ellipticity for ultracold polar molecules

Microwave(MW) fields with strong field strength, ultralow phase-noise and tunable polarization are crucial for stabilizing and manipulating ultracold polar molecules, which have emerged as a promising platform for quantum sciences. In this letter, we present the design, characterization, and performance of a robust MW setup tailored for precise control of molecular states. This setup achieves a high electric field intensity of 6.9 kV/m in the near-field from a dual-feed waveguide antenna, enabling a Rabi frequency as high as 71 MHz for the rotational transition of sodium-potassium molecules. In addition, the low noise signal source and controlled electronics provide ultralow phase-noise and dynamically tunable polarization. Narrow-band filters within the MW circuitry further reduce phase-noise by more than 20 dB at 20 MHz offset frequency, ensuring prolonged one-body molecular lifetimes up to 10 seconds. We also show practical methods to measure the MW field strength and polarization using a simple homemade dipole probe, and to characterize phase-noise down to -170 dBc/Hz with a commercial spectrum analyser and a notch filter. Those capabilities allowed us to evaporatively cool our molecular sample to deep quantum degeneracy. Furthermore, the polarization tunability enabled the observation of field-linked resonances and facilitated the creation of field-linked tetramers.These techniques advance the study of ultracold polar molecules and broaden the potential applications of MW tools in other platforms of quantum sciences.

physics.atom-ph

Numerical modeling of laser cooling in molecules: From simple diatomics to polyatomics and radioactive species

Optical Bloch equations and rate equations serve as powerful tools to model light-matter interactions from textbook-like two-level atoms to the complex internal dynamics of molecules. A particular challenge in this context is posed by molecular laser cooling, where many dozens or hundreds of levels need to be taken into account for a comprehensive modeling. Here, we present MoleCool, a numerically efficient Python toolbox to implement and solve the corresponding differential equation systems. We illustrate both the capabilities of the toolbox and some of the intricacies of molecular laser cooling by educational examples, which range from simple Rabi oscillations to spontaneous and coherent cooling schemes for various currently studied or considered molecular species. This includes, in particular, a comprehensive modeling of laser cooling dynamics with full hyperfine structure resolution in radioactive radium monofluoride (RaF), as well as studies of other complex species such as barium monofluoride (BaF) and ytterbium monohydroxide (YbOH).

physics.atom-ph

Tunable Field-Linked $s$-wave Interactions in Dipolar Fermi Mixtures

Spin mixtures of degenerate fermions are a cornerstone of quantum many-body physics, enabling superfluidity, polarons, and rich spin dynamics through $s$-wave scattering resonances. Combining them with strong, long-range dipolar interactions provides highly flexible control schemes promising even more exotic quantum phases. Recently, microwave shielding gave access to spin-polarized degenerate samples of dipolar fermionic molecules, where tunable $p$-wave interactions were enabled by field-linked resonances available only by compromising the shielding. Here, we study the scattering properties of a fermionic dipolar spin mixture and show that a universal $s$-wave resonance is readily accessible without compromising the shielding. We develop a universal description of the tunable $s$-wave interaction and weakly bound tetratomic states based on the microwave-field parameters. The $s$-wave resonance paves the way to stable, controllable and strongly-interacting dipolar spin mixtures of deeply degenerate fermions and supports favorable conditions to reach this regime via evaporative cooling.

cond-mat.quant-gas

Ultracold field-linked tetratomic molecules

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.

cond-mat.quant-gas

Ultracold Sticky Collisions: Theoretical and Experimental Status

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.

physics.chem-ph

Field-linked resonances of polar molecules

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.

cond-mat.quant-gas

Observation of confinement-induced resonances in a 3D lattice

We report on the observation of confinement-induced resonances for strong three-dimensional (3D) confinement in a lattice potential. Starting from a Mott-insulator state with predominantly single-site occupancy, we detect loss and heating features at specific values for the confinement length and the 3D scattering length. Two independent models, based on the coupling between the center-of-mass and the relative motion of the particles as mediated by the lattice, predict the resonance positions to a good approximation, suggesting a universal behavior. Our results extend confinement-induced resonances to any dimensionality and open up an alternative method for interaction tuning and controlled molecule formation under strong 3D confinement.

cond-mat.quant-gas

Suppression of Unitary Three-body Loss in a Degenerate Bose-Fermi Mixture

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.

cond-mat.quant-gas

Long-lived fermionic Feshbach molecules with tunable $p$-wave interactions

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.

cond-mat.quant-gas

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 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.

cond-mat.quant-gas

Transition from a polaronic condensate to a degenerate Fermi gas of heteronuclear molecules

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.

cond-mat.quant-gas

Efficient conversion of closed-channel dominated Feshbach molecules of $^{23}$Na$^{40}$K to their absolute ground state

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 $|c^3 Σ^+, v=35, J=1 \rangle \sim |B^1Π, v=12, J=1\rangle$. 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.

cond-mat.quant-gas

Collisions of ultracold molecules in bright and dark optical dipole traps

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.

cond-mat.quant-gas