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Atoms

Universal Scattering of Ultracold Atoms and Molecules in Optical Potentials

Hui Li, Ming Li, Constantinos Makrides, Alexander N. Petrov, Svetlana Kotochigova

Published Mar 15, 2019• 15 citations
Publisher

Abstract

Universal collisions describe the reaction of molecules and atoms as dominated by long-range interparticle interactions. Here, we calculate the universal inelastic rate coefficients for a large group of ultracold polar molecules in their lower ro-vibrational states colliding with one of their constituent atoms. The rate coefficients are solely determined by values of the dispersion coefficient and reduced mass of the collisional system. We use the ab initio coupled-cluster linear response method to compute dynamic molecular polarizabilities and obtain the dispersion coefficients for some of the collisional partners and use values from the literature for others. Our polarizability calculations agree well with available experimental measurements. Comparison of our inelastic rate coefficients with results of numerically exact quantum-mechanical calculations leads us to conjecture that collisions with heavier atoms can be expected to be more universal.

DOI
10.3390/atoms7010036

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Universal collisions describe the reaction of molecules and atoms as dominated by long-range interparticle interactions. Here, we calculate the universal inelastic rate coefficients for a large group of ultracold polar molecules in their lower ro-vibrational states colliding with one of their constituent atoms. The rate coefficients are solely determined by values of the dispersion coefficient and reduced mass of the collisional system. We use the ab initio coupled-cluster linear response method to compute dynamic molecular polarizabilities and obtain the dispersion coefficients for some of the collisional partners and use values from the literature for others. Our polarizability calculations agree well with available experimental measurements. Comparison of our inelastic rate coefficients with results of numerically exact quantum-mechanical calculations leads us to conjecture that collisions with heavier atoms can be expected to be more universal.
Progress in ultracold experiments with polar molecules requires a clear understanding of their interactions and reactivity at ultralow collisional energies. Two important theoretical steps in this process are the characterization of interaction potentials between molecules and the modeling of the reactive scattering mechanism. Here, we report on the ab initio calculation of isotropic and anisotropic van der Waals interaction potentials for polar KRb and RbCs colliding with each other or with ultracold atoms. Based on these potentials and two short-range scattering parameters, we then develop a single-channel scattering model with flexible boundary conditions. Our calculations show that, at low temperatures (and in the absence of an external electric field), the reaction rates between molecules or between molecules and atoms have a resonant character as a function of the short-range parameters. We also find that both the isotropic and anisotropic van der Waals coefficients have significant contributions from dipole coupling to excited electronic states. Their values can differ dramatically from those solely obtained from the permanent dipole moment. A comparison with recently obtained reaction rates of fermionic 40 K 87 Rb shows that the experimental data cannot be explained by a model where the short-range scattering parameters are independent of the relative orbital angular momentum or partial wave.
Universal collision rate constants are calculated for ultracold collisions of two like bosonic or fermionic heteronuclear alkali-metal dimers involving the species Li, Na, K, Rb, or Cs. Universal collisions are those for which the short range probability of a reactive or quenching collision is unity such that a collision removes a pair of molecules from the sample. In this case, the collision rates are determined by universal quantum dynamics at very long range compared to the chemical bond length. We calculate the universal rate constants for reaction of the reactive dimers in their ground vibrational state v = 0 and for vibrational quenching of non-reactive dimers with v ≥ 1. Using the known dipole moments and estimated van der Waals coefficients of each species, we calculate electric field dependent loss rate constants for collisions of molecules tightly confined to quasi-two-dimensional geometry by a one-dimensional optical lattice. A simple scaling relation of the quasi-two-dimensional loss rate constants with dipole strength, trap frequency and collision energy is given for like bosons or like fermions. It should be possible to stabilize ultracold dimers of any of these species against destructive collisions by confining them in a lattice and orienting them with an electric field of less than 20 kV cm(-1).
In this thesis properties of ultracold alkali dimers are studied both theoretically and experimentally. In the first, theoretical, part, the prospects for the formation of ultracold LiCs dimers in deeply bound vibrational levels using photoassociation (PA) are investigated. Furthermore a previous systematic investigation of the structure of all alkali dimers is extended by the ab initio calculation of static dipole polarizabilities. An extensive comparison with other published results supports the reliability of the chosen method. Based on these results an experimental scheme for the creation of an sample of oriented ultracold dipolar molecules is developed. In the second, experimental part the formation of LiCs ground state molecules by PA is investigated. PA spectroscopy is used to improve the accuracy of the potential energy curve for the B1P and the value of the dissociation energy of the X1S+ state significantly. The rovibrational distribution of ground state molecules is probed in a combination of resonance-enhanced multi-photon ionization and depletion spectroscopy. A simple scheme is found to form ultracold polar LiCs molecules in the absolute ground state X1S+,v''=0,J''=0. In a quasi-electrostatic trap created by a CO2 laser, LiCs molecules are formed and stored. A lifetime of 24(3)s, limited by collisions with background gas, is observed and rate coefficients for inelastic collisions between LiCs in high vibrational states and Cs atoms are determined. The long storage time facilitates the observation of radiative decay of polar molecules towards lower vibrational levels.
The coefficients at the lowest-order electrostatic, induction, and dispersion terms of the anisotropic long-range potential between the two KRb((1)Σ(+)) molecules are evaluated through the static and dynamic molecular properties using the ab initio coupled cluster techniques. Adiabatic channel potentials for the ground-state molecules are obtained and used for the numerical quantum capture probability calculations in the spirit of the statistical adiabatic channel models. Capture rate coefficients for indistinguishable (polarized) and distinguishable (unpolarized) molecules at temperatures below 10 μK agree well with those computed with the simple isotropic dispersion R(-6) potential, but underestimate the measured ones [Ospelkaus et al., Science 327, 853 (2010)] up to a factor of 3. Preliminary assessment of the effects of higher-order long-range terms, retardation of dispersion forces, and magnetic dipole-dipole interaction does not offer any clear perspectives for drastic improvement of the capture approximation for the reactions studied.
We consider ultracold collisions of ground-state heteronuclear alkali-metal dimers that are susceptible to four-center chemical reactions $2AB\ensuremath{\rightarrow}{A}_{2}+{B}_{2}$ even at submicrokelvin temperatures. These reactions depend strongly on species, temperature, electric field, and confinement in an optical lattice. We calculate ab initio van der Waals coefficients for these interactions and use a quantum formalism to study the scattering properties of such molecules under an external electric field and optical lattice. We also apply a quantum threshold model to explore the dependence of reaction rates on the various parameters. We find that, among the heteronuclear alkali-metal fermionic species, LiNa is the least reactive, whereas LiCs is the most reactive. For the bosonic species, LiK is the most reactive in zero field, but all species considered, LiNa, LiK, LiRb, LiCs, and KRb, share a universal reaction rate once a sufficiently high electric field is applied. For indistinguishable bosons, the inelastic/reactive rate increases as d2{d}^{2}d2 in the quantum regime, where ddd is the dipole moment induced by the electric field. This is a weaker power-law dependence than for indistinguishable fermions, for which the rate behaves as d6{d}^{6}d6.