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Physica Scripta

Field-Linked States in Ultracold Molecular Collisions

John L. Bohn, А. V. Avdeenkov

Published Jan 1, 2004• 1 citation
Publisher

Abstract

At ultralow temperatures, and in the presence of an electric field, the long-range interaction potentials between dipolar molecules are highly subject to manipulation. Most strikingly, a novel set of quasi-bound states, dubbed "field-linked" states, appear. In these states the molecules are held at intermolecular distances of tens to hundreds of atomic units, and can strongly influence resonant scattering of molecules.

DOI
10.1238/physica.topical.110a00292

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At ultralow temperatures, and in the presence of an electric field, the long-range interaction potentials between dipolar molecules are highly subject to manipulation. Most strikingly, a novel set of quasi-bound states, dubbed "field-linked" states, appear. In these states the molecules are held at intermolecular distances of tens to hundreds of atomic units, and can strongly influence resonant scattering of molecules.
We explore the character of a novel set of ``field-linked'' states that were predicted by Avdeenkov and Bohn [Phys. Rev. Lett. 90, 043006 (2003)]. These states exist at ultralow temperatures in the presence of an electrostatic field, and their properties are strongly dependent on the field's strength. We clarify the nature of these quasibound states by constructing their wave functions and determining their approximate quantum numbers. As the properties of field-linked states are strongly defined by anisotropic dipolar and Stark interactions, we construct adiabatic surfaces as functions of both the intermolecular distance and the angle that the intermolecular axis makes with the electric field. Within an adiabatic approximation we solve the two-dimensional Schr\"odinger equation to find bound states, whose energies correlate well with resonance features found in fully converged multichannel scattering calculations.
The presence of electric or microwave fields can modify the long-range forces between ultracold dipolar molecules in such a way as to engineer weakly bound states of molecule pairs. These so-called field-linked states [A. V. Avdeenkov and J. L. Bohn, Phys. Rev. Lett. 90, 043006 (2003).PRLTAO0031-900710.1103/PhysRevLett.90.043006; L. Lassablière and G. Quéméner, Phys. Rev. Lett. 121, 163402 (2018).PRLTAO0031-900710.1103/PhysRevLett.121.163402], in which the separation between the two bound molecules can be orders of magnitude larger than the molecules themselves, have been observed as resonances in scattering experiments [X.-Y. Chen et al., Nature (London) 614, 59 (2023).NATUAS0028-083610.1038/s41586-022-05651-8]. Here, we propose to use them as tools for the assembly of weakly bound tetramer molecules, by means of ramping an electric field, the electric-field analog of magnetoassociation in atoms. This ability would present new possibilities for constructing ultracold polyatomic molecules.
We predict the existence of stable bound states between pairs of ultracold diatomic molecules with the aid of a static electric field and 1D harmonic confinement. We focus on collisions of NaK-NaK identical fermions, for which we find that currently achievable experimental parameters allow the observation of these confinement-induced field-linked bound states as scattering resonances. The bound state is highly stable with lifetimes estimated to be tens of seconds long. With the diatomic molecules bound at distances a fraction of the dipolar length scale, these complexes allow for explorations of polyatomic chemistry and Fermi gas superfluid pairing.
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
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 predict that pairs of polar molecules can be weakly bound together in an ultracold environment, provided that a dc electric field is present. The field that links the molecules together also strongly influences the basic properties of the resulting dimer, such as its binding energy and predissociation lifetime. Because of their long-range character, these dimers will be useful in disentangling cold collision dynamics of polar molecules. As an example, we estimate the microwave photoassociation yield for OH-OH cold collisions.