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arXiv:2009.07461 · Science

Resonant collisional shielding of reactive molecules using electric fields

Kyle Matsuda, Luigi De Marco, Jun-Ru Li, William G. Tobias, Giacomo Valtolina, Goulven Quéméner, Jun Ye

Published Dec 10, 2020• 121 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1126/science.abe7370

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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.
Ultracold Chemistry Because reactive collisions limit the lifetime of ultracold molecular ensembles, controlling chemical reactivity at ultralow temperatures has been a long-standing goal. Using large electric fields that trigger resonant dipolar interactions between potassium-rubidium molecules trapped in a quasi–two-dimensional geometry, Matsuda et al. report suppression of the reactive loss rate in the vicinity of the dipolar-mediated resonances by up to an order of magnitude below the background value. The proposed shielding mechanism is general and is expected to be effective in three-dimensional geometry. It could also be used for creating long-lived quantum molecular gases of other polar molecules under strong electric fields. Science , this issue p. [1324][1] [1]: /lookup/doi/10.1126/science.abe7370
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.
Ultracold polar molecules possess long-range, anisotropic, and tunable dipolar interactions, providing unique opportunities to probe novel quantum phenomena. However, experimental progress has been hindered by excessive two-body loss, which also limits further cooling via evaporation. Recent work shows the loss can be mitigated by confining molecules in a two-dimensional geometry. However, a general approach for tuning molecular interactions in a full three-dimensional (3D) stable system has been lacking. Here, we demonstrate the use of an electric field-induced shielding resonance to suppress the reactive loss by a factor of 30 while preserving elastic, long-range dipolar interactions in a bulk gas of ultracold 40K87Rb molecules in 3D. The favorable ratio of elastic to inelastic collisions enables direct thermalization, the rate of which depends on the angle between the collisional axis and the dipole orientation controlled by an external electric field. This is a direct manifestation of the anisotropic dipolar interaction. We further achieve dipolar-interaction-mediated evaporative cooling in 3D. This work demonstrates control of a long-lived bulk quantum gas system with tunable long-range interactions, paving the way for the study of collective quantum many-body physics.
The prospects for shielding ultracold, paramagnetic, dipolar molecules from inelastic and chemical collisions are investigated. Molecules placed in their first rotationally excited states are found to exhibit effective long-range repulsion for applied electric fields above a certain critical value, as previously shown for nonparamagnetic molecules. This repulsion can safely allow the molecules to scatter while reducing the risk of inelastic or chemically reactive collisions. Several molecular species of $^{2}\mathrm{\ensuremath{\Sigma}}$ molecules of experimental interest---RbSr, SrF, BaF, and YO---are considered, and all are shown to exhibit orders of magnitude suppression in quenching rates in a sufficiently strong laboratory electric field. It is further shown that, for these molecules described by Hund's coupling case (b), electronic and nuclear spins play the role of spectator with respect to the shielding.
Microscopic control over polar molecules with tunable interactions enables the realization of distinct quantum phenomena. Using an electric field gradient, we demonstrated layer-resolved state preparation and imaging of ultracold potassium-rubidium molecules confined to two-dimensional planes in an optical lattice. The rotational coherence was maximized by rotating the electric field relative to the light polarization for state-insensitive trapping. Spatially separated molecules in adjacent layers interact through dipolar spin exchange of rotational angular momentum; by adjusting these interactions, we regulated the local chemical reaction rate. The resonance width of the exchange process vastly exceeded the dipolar interaction energy, an effect attributed to thermal energy. This work realized precise control of interacting molecules, enabling electric field microscopy on subwavelength scales and allowing access to unexplored physics in two-dimensional systems.
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 23Na40K^{23}\mathrm{Na}^{40}\mathrm{K}23Na40K and bosonic 23Na39K^{23}\mathrm{Na}^{39}\mathrm{K}23Na39K molecules.