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arXiv:2407.04901 · Physical Review Letters

Three-Body Recombination of Ultracold Microwave-Shielded Polar Molecules

Ian Stevenson, Shayamal Singh, Ahmed A. Elkamshishy, Niccolò Bigagli, Weijun Yuan, Siwei Zhang, Chris H. Greene, Sebastian Will

Published Dec 24, 2024• 16 citations
arXivHTMLPDF

Abstract

A combined experimental and theoretical study is carried out on the three-body recombination process in a gas of microwave-shielded polar molecules. For ground-state polar molecules dressed with a strong microwave field, field-linked bound states can appear in the intermolecular potential. We model three-body recombination into such bound states using classical trajectory calculations. Our results show that recombination can explain the enhanced loss rates observed at small microwave detunings in trapped samples of bosonic NaCs [Bigagli et al., Nat. Phys. 19, 1579-1584 (2023)NPAHAX1745-247310.1038/s41567-023-02200-6]. Specifically, our calculations reproduce the experimentally measured three-body loss rates across a wide range of microwave Rabi couplings, detunings, and temperatures. This work suggests that for bosonic shielded molecular systems in which the two-body loss is sufficiently suppressed and a field-linked bound state is present, the dominant loss process will be three-body recombination.

DOI
10.1103/physrevlett.133.263402

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A combined experimental and theoretical study is carried out on the three-body recombination process in a gas of microwave-shielded polar molecules. For ground-state polar molecules dressed with a strong microwave field, field-linked bound states can appear in the intermolecular potential. We model three-body recombination into such bound states using classical trajectory calculations. Our results show that recombination can explain the enhanced loss rates observed at small microwave detunings in trapped samples of bosonic NaCs [Bigagli et al., Nat. Phys. 19, 1579-1584 (2023)NPAHAX1745-247310.1038/s41567-023-02200-6]. Specifically, our calculations reproduce the experimentally measured three-body loss rates across a wide range of microwave Rabi couplings, detunings, and temperatures. This work suggests that for bosonic shielded molecular systems in which the two-body loss is sufficiently suppressed and a field-linked bound state is present, the dominant loss process will be three-body recombination.
We develop double microwave shielding, which has recently enabled evaporative cooling to the first Bose-Einstein condensate of polar molecules [Bigagli , Nature , 289 (2024)]. Two microwave fields of different frequency and polarization are employed to effectively shield polar molecules from inelastic collisions and three-body recombination. Here, we describe in detail the theory of double microwave shielding. We demonstrate that double microwave shielding effectively suppresses two- and three-body losses. Simultaneously, dipolar interactions and the scattering length can be flexibly tuned, enabling comprehensive control over interactions in ultracold gases of polar molecules. We show that this approach works universally for a wide range of molecules. This opens the door to studying many-body physics with strongly interacting dipolar quantum matter.
Microwave shielding is an important technique that can suppress the losses that arise from collisions of ultracold polar molecules. It has been instrumental in achieving molecular Bose-Einstein condensation (BEC) for NaCs []. We demonstrate that microwave shielding is universal, in the sense that the two-body collision properties of different molecules are very similar when expressed in suitable reduced units of length and energy. This applies to rate coefficients for inelastic scattering and loss, to scattering lengths, and to the properties of two-molecule bound states. We also explore the small deviations from universality that arise at very large Rabi frequencies. In general, the collision properties are near-universal except when the Rabi frequency exceeds a few percent of the molecular rotational constant. The universality extends to elliptically polarized microwaves and to combinations of multiple fields. Our results indicate that the methods that have been used to achieve BEC for NaCs can be transferred directly to most other polar molecules.
The ability to tune interparticle interactions is one of the main advantages of using ultracold quantum gases for quantum simulation of many-body physics. Current experiments with ultracold polar molecules employ shielding with microwave or static electric fields to prevent destructive collisional losses. The interaction potential of microwave-shielded molecules can be tuned by using microwaves of two different polarisations, while for static-field-shielded molecules the tunability of interactions is more limited and depends on the particular species. In this work, we propose a general method to tune the interactions between static-field-shielded molecules by applying a microwave field. We carry out coupled-channel scattering calculations in a field-dressed basis set to determine loss rate coefficients and scattering lengths. We find that both the s-wave scattering length and the dipole length can be widely tuned by changing the parameters of the microwave field, while maintaining strong suppression of lossy collisions.
We propose a method to suppress collisional loss in strongly dipolar, rotationally excited ultracold molecules using a combination of static (dc) and microwave (ac) electric fields. By tuning two excited pair molecular rotational states into a Förster resonance with a dc field, simultaneously driving excited rotational transitions with an ac field removes all long-range bound states, allowing near complete suppression of all two- and three-body collisional loss channels. While permitting tunable dipolar and anti-dipolar interactions, this bound-state-free ac/dc scheme is not subject to photon-changing collisions that are the primary source of two-body loss in shielding with two microwave fields, used to achieve the first molecular Bose-Einstein condensate [Bigagli et al., Nature 631, 289 (2024)]. Using NaCs as a representative example for strongly dipolar molecules, close-coupling calculations are performed to show that bound-state-free shielding can achieve ratios of elastic-to-loss rates ≳106\gtrsim 10^{6}≳106 at 100 nK, with currently accessible ac and dc field generation technologies. This work opens new opportunities for realizing large, long-lived samples of strongly interacting degenerate molecular gases with tunable long-range interactions.
We report on the optical polarizability of microwave-shielded ultracold NaCs molecules in an optical dipole trap. While dressing a pair of rotational states with a microwave field, we observe a marked dependence of the optical polarizability on the intensity and detuning of the dressing field. To precisely characterize differential energy shifts between dressed rotational states, we establish dressed-state spectroscopy. For strong dressing fields, we find that a magic rotational transition can be engineered and demonstrate its insensitivity to laser intensity fluctuations. The results of this Letter have direct relevance for evaporative cooling and the recent demonstration of molecular Bose-Einstein condensates [Bigagli et al., Nature (London) 631, 289 (2024)NATUAS0028-083610.1038/s41586-024-07492-z] and may open a door to precision microwave spectroscopy in interacting many-body systems of microwave-shielded molecules.
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.