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arXiv:2106.01610 · Physical Review A

Resonant and first-order dipolar interactions between ultracold Σ 1 molecules in static and microwave electric fields

Tijs Karman, Zoe Z. Yan, Martin W. Zwierlein

Published Jan 28, 2022• 21 citations
arXivHTMLPDF

Abstract

We theoretically study collisions between ultracold polar $^{1}\mathrm{\ensuremath{\Sigma}}$ molecules that are polarized by microwave or static electric fields. We systematically study the dependence on field strength, microwave polarization, and detuning from rotational transitions. We calculate the loss in two-body collisions that is observable experimentally and compare with the results expected for purely first-order dipolar interactions. For ground-state molecules polarized by a static electric field, the dynamics are accurately described by first-order dipolar interactions. For microwave dressing, instead, resonant dipolar collisions dominate the collision process, in which molecules reorient along the intermolecular axis and interact with the full strength of the transition dipole. For red detuning, reorientation can only be suppressed at extreme Rabi frequencies. For blue detuned microwaves, resonant dipolar interactions dominate even for the highest Rabi frequencies, leading to microwave shielding for circular polarization and structured losses due to resonances for linear polarization. The results are presented numerically for fermionic $^{23}\mathrm{Na}^{40}\mathrm{K}$ and bosonic $^{23}\mathrm{Na}^{39}\mathrm{K}$ molecules.

DOI
10.1103/physreva.105.013321

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Collisions at ultracold temperatures between ${}^{1}\phantom{\rule{-0.16em}{0ex}}\ensuremath{\Sigma}$-state diatomic polar molecules in a circularly polarized microwave field are theoretically analyzed. We demonstrate that elastic and inelastic collisions of polar molecules at ultracold temperatures are affected by an external microwave field and that they are enhanced at resonance frequencies. We show that the collision dynamics of polar molecules in a microwave field is largely determined by the long-range dipole-dipole interaction. Through this interaction, two polar molecules can resonantly exchange internal energy by undergoing a transition between neighboring rotational levels. This process may stabilize the system and enable the successive evaporative cooling of molecules. This paper discusses fermionic polar molecules at ultralow temperatures (1 $\ensuremath{\mu}$K).
We demonstrate microwave dressing on ultracold, fermionic ^{23}Na^{40}K ground-state molecules and observe resonant dipolar collisions with cross sections exceeding 3 times the s-wave unitarity limit. The origin of these interactions is the resonant alignment of the approaching molecules' dipoles along the intermolecular axis, which leads to strong attraction. We explain our observations with a conceptually simple two-state picture based on the Condon approximation. Furthermore, we perform coupled-channel calculations that agree well with the experimentally observed collision rates. The resonant microwave-induced collisions found here enable controlled, strong interactions between molecules, of immediate use for experiments in optical lattices.
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.
Full control of molecular interactions, including reactive losses, would open new frontiers in quantum science. We demonstrate extreme tunability of ultracold chemical reaction rates by inducing resonant dipolar interactions by means of an external electric field. We prepared fermionic potassium-rubidium molecules in their first excited rotational state and observed a modulation of the chemical reaction rate by three orders of magnitude as we tuned the electric field strength by a few percent across resonance. In a quasi-two-dimensional geometry, we accurately determined the contributions from the three dominant angular momentum projections of the collisions. Using the resonant features, we shielded the molecules from loss and suppressed the reaction rate by an order of magnitude below the background value, thereby realizing a long-lived sample of polar molecules in large electric fields.
The dipolar collision between ultracold polar molecules is an important topic both by its own right from the fundamental point of view and for the successful exploration of many-body physics with strong and longrange dipolar interactions.Here, we report the investigation of collisions between ultracold ground-state sodium-rubidium molecules in electric fields with induced electric dipole moments as large as 0.7 D. We observe a stepwise enhancement of losses due to the coupling between different partial waves induced by the increasingly stronger anisotropic dipolar interactions.Varying the temperature of our sample, we find good agreement with theoretical loss rates assuming complex formation as the main loss process.Our results shed new light on the understanding of complex molecular collisions in the presence of strong dipolar interactions and also demonstrate the versatility of modifying molecular interactions with electric fields.