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arXiv:2305.07600 · Physical Review Research

Shielding collisions of ultracold CaF molecules with static electric fields

Bijit Mukherjee, Matthew D. Frye, C. Ruth Le Sueur, Michael R. Tarbutt, Jeremy M. Hutson

Published Aug 10, 2023• 15 citations
arXivHTMLPDF

Abstract

We study collisions of ultracold CaF molecules in strong static electric fields. These fields allow the creation of long-range barriers in the interaction potential, effectively preventing the molecules from reaching the short-range region where inelastic and other loss processes are likely to occur. We carry out coupled-channel calculations of rate coefficients for elastic scattering and loss. We develop an efficient procedure for including energetically well-separated rotor functions in the basis set via a Van Vleck transformation. We show that shielding is particularly efficient for CaF and allows the rate of two-body loss processes to be reduced by a factor of ${10}^{7}$ or more at a field of 23 kV/cm. The loss rates remain low over a substantial range of fields. Electron and nuclear spins cause strong additional loss in some small ranges of field, but have little effect elsewhere. These results pave the way for evaporative cooling of CaF towards quantum degeneracy.

DOI
10.1103/physrevresearch.5.033097

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We study collisions of ultracold CaF molecules in strong static electric fields. These fields allow the creation of long-range barriers in the interaction potential, effectively preventing the molecules from reaching the short-range region where inelastic and other loss processes are likely to occur. We carry out coupled-channel calculations of rate coefficients for elastic scattering and loss. We develop an efficient procedure for including energetically well-separated rotor functions in the basis set via a Van Vleck transformation. We show that shielding is particularly efficient for CaF and allows the rate of two-body loss processes to be reduced by a factor of 107{10}^{7}107 or more at a field of 23 kV/cm. The loss rates remain low over a substantial range of fields. Electron and nuclear spins cause strong additional loss in some small ranges of field, but have little effect elsewhere. These results pave the way for evaporative cooling of CaF towards quantum degeneracy.
The strong, tunable dipolar interactions of ultracold molecules make them a powerful platform for quantum many-body physics, but reaching degeneracy by evaporative cooling requires suppressing inelastic collisions. Microwave collisional shielding has enabled the preparation of degenerate Fermi gases and Bose-Einstein condensates of polar molecules, whereas static electric field shielding has been limited to fermionic species, which are less prone to inelastic loss. We demonstrate static-field Förster shielding of bosonic 23^{23}23Na87^{87}87Rb molecules, suppressing two-body loss by up to four orders of magnitude. Within a bound-state-free electric-field window, three-body loss is also strongly suppressed, enabling efficient evaporation. Evaporating with an efficiency of 2.09(9), we increase the phase-space density of the gas by two orders of magnitude, reaching degeneracy with 7200(1000) molecules. We observe self-bound droplets at the end of evaporation over a wide range of field strengths, emerging from either degenerate or non-degenerate parent gases. We perform Path Integral Monte Carlo simulations, which suggest that the observed droplets are filamentary in nature, and find good agreement with the experimentally observed droplet formation temperatures. Our results establish Förster shielding as a single-field route to prepare degenerate gases and self-bound droplets of bosonic polar molecules.
Trapped samples of ultracold molecules are often short-lived because close collisions between them result in trap loss. We investigate the use of shielding with static electric fields to create repulsive barriers between polar molecules to prevent such loss. Shielding is very effective even for RbCs, with a relatively low dipole moment, and even more effective for molecules such as NaK, NaRb, and NaCs, with progressively larger dipoles. Varying the electric field allows substantial control over the scattering length, which will be crucial for the stability or collapse of molecular Bose-Einstein condensates. This arises because the dipole-dipole interaction creates a long-range attraction that is tunable with electric field. For RbCs, the scattering length is positive across the range where shielding is effective because the repulsion responsible for shielding dominates. For NaK, the scattering length can be tuned across zero to negative values. For NaRb and NaCs, the attraction is strong enough to support tetra-atomic bound states, and the scattering length passes through resonant poles where these states cross threshold. For KAg and CsAg, there are multiple bound states and multiple poles. For each molecule, we calculate the variation of the scattering length with field and comment on the possibilities for exploring new physics. Published by the American Physical Society 2024
Harnessing the potential wide-ranging quantum science applications of molecules will require control of their interactions. Here, we used microwave radiation to directly engineer and tune the interaction potentials between ultracold calcium monofluoride (CaF) molecules. By merging two optical tweezers, each containing a single molecule, we probed collisions in three dimensions. The correct combination of microwave frequency and power created an effective repulsive shield, which suppressed the inelastic loss rate by a factor of six, in agreement with theoretical calculations. The demonstrated microwave shielding shows a general route to the creation of long-lived, dense samples of ultracold polar molecules and evaporative cooling.
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.
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.
Long range intermolecular interaction potential surface of CaF ( 2 Σ + ) was simulated by employing the MOLPRO program and using the RCCSD(T)/def2-TZVP theory. The predicted data were further fitted to obtain the collision cross-section. The elastic collision cross-section of CaF at the temperature around 2 mK is as high as 6.5×10 −9 cm 2 and the collision rate is over 4.1×10 6 Hz. Additionally, we found that an orientation electric field will simplify the intermolecular interaction potential function from quaternary into ternary and the collision cross-section will be raised by about three orders. All-optical evaporative cooling of cold CaF is discussed in the conclusion.