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arXiv:2405.13645

Formation and Dissociation of Field-Linked Tetramers

Fulin Deng, Xing-Yan Chen, Xinyu Luo, Wenxian Zhang, Su Yi, Shi, Tao

Published May 22, 2024• 1 citation
arXivHTMLPDF

Abstract

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.

DOI
10.48550/arxiv.2405.13645

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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.
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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.
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Abstract Scattering resonances are an essential tool for controlling the interactions of ultracold atoms and molecules. However, conventional Feshbach scattering resonances 1 , which have been extensively studied in various platforms 1–7 , are not expected to exist in most ultracold polar molecules because of the fast loss that occurs when two molecules approach at a close distance 8–10 . Here we demonstrate a new type of scattering resonance that is universal for a wide range of polar molecules. The so-called field-linked resonances 11–14 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 superfluids 15 and molecular supersolids 16 , as well as assembling ultracold polyatomic molecules.
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.
Double microwave shielding employs σ+σ^{+}σ+- and πππ-polarized microwave fields, tuned close to the lowest rotational transition, to engineer a long-range repulsive barrier between polar molecules. By preventing molecules from reaching the short range, this technique suppresses detrimental two-body losses and recently enabled the realization of molecular Bose-Einstein condensates and self-bound droplets. Yet, the optimal operating regimes of the shielding mechanism remain largely unexplored. Here, by leveraging the underlying universality of the scattering problem, we systematically map the four-dimensional microwave parameter space-spanned by the detunings and intensities of the two fields-to identify configurations that maximize both shielding efficiency and interaction tunability. We define optimal operating regimes as configurations that are strictly free of field-linked bound states while sufficiently suppressing two-body losses to exceed typical lifetimes of ultracold samples. In these regimes, we evaluate the elastic-to-inelastic collision ratios required for efficient evaporative cooling and explore the accessible tuning range of the effective dipolar interactions. Finally, to identify the best platforms for future quantum simulation experiments, we conduct a global survey of candidate molecular species under realistic field constraints. We identify heavy, strongly dipolar molecules as the most promising candidates, demonstrating that they can achieve extreme loss suppression-reaching two-body loss rates as low as 10−1810^{-18}10−18 cm3^{3}3/s-alongside robust interaction tunability using only moderate field strengths.