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Physical Review A

Collision-induced spin exchange of alkali-metal atoms with H3e : Anab initiostudy

Timur V. Tscherbul, P. Zhang, H. R. Sadeghpour, A. Dalgarno

Published Jun 9, 2009• 25 citations
Publisher

Abstract

We present a rigorous quantum study of spin-exchange transitions in collisions of the alkali-metal atoms with $^{3}\text{H}\text{e}$ in the presence of an external magnetic field. Using accurate ab initio interaction potentials, we obtain refined estimates for the Fermi contact interaction constants for complexes of Na, K, and Rb atoms with $^{3}\text{H}\text{e}$. Ab initio calculations show that the Fermi contact interaction in $\text{Li-}^{3}\text{H}\text{e}$ varies more slowly with internuclear distance than predicted by the atomic model [R. M. Herman, Phys. Rev. 37, A1062 (1965)]. The calculated spin-exchange rate constants for Na, K, and Rb atoms in a gas of $^{3}\text{H}\text{e}$ are in good agreement with experimental data. Our calculations demonstrate that at a temperature of 0.5 K, collision-induced spin exchange of the alkali-metal atoms occurs at a very slow rate of $\ensuremath{\sim}{10}^{\ensuremath{-}22}\text{ }{\text{cm}}^{3}/\text{s}$, suggesting potential applications in cryogenic cooling, precision spectroscopy, and quantum optics.

DOI
10.1103/physreva.79.062707

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We present a rigorous quantum study of spin-exchange transitions in collisions of the alkali-metal atoms with 3He^{3}\text{H}\text{e}3He in the presence of an external magnetic field. Using accurate ab initio interaction potentials, we obtain refined estimates for the Fermi contact interaction constants for complexes of Na, K, and Rb atoms with 3He^{3}\text{H}\text{e}3He. Ab initio calculations show that the Fermi contact interaction in Li-3He\text{Li-}^{3}\text{H}\text{e}Li-3He varies more slowly with internuclear distance than predicted by the atomic model [R. M. Herman, Phys. Rev. 37, A1062 (1965)]. The calculated spin-exchange rate constants for Na, K, and Rb atoms in a gas of 3He^{3}\text{H}\text{e}3He are in good agreement with experimental data. Our calculations demonstrate that at a temperature of 0.5 K, collision-induced spin exchange of the alkali-metal atoms occurs at a very slow rate of \ensuremath∼10\ensuremath−22 cm3/s\ensuremath{\sim}{10}^{\ensuremath{-}22}\text{ }{\text{cm}}^{3}/\text{s}\ensuremath∼10\ensuremath−22 cm3/s, suggesting potential applications in cryogenic cooling, precision spectroscopy, and quantum optics.
Collisions of atoms and molecules in external electromagnetic fields can depolarize electronic and nuclear spins, leading to decoherence of quantum superposition states. The fundamental microscopic processes giving rise to spin depolarization are spin exchange and spin relaxation. In this work, we present an analysis of spin exchange transitions in collision of alkali metal atoms with 3He. We use accurate ab initio calculations to evaluate the electron spin density of Li-He and the interaction energy of Rb-He. The Fermi contact interaction constants for the complexes of Na, K, and Rb atoms with 3He are extracted from the measured frequency shift enhancement factors using the ab initio interaction potentials. The spin density calculations also yield the hyperfine pressure shift of Li-He.
We present a joint experimental and theoretical study of spin depolarization in collisions of alkali-metal atoms with 3He^{3}\mathrm{He}3He in a magnetic field. A rigorous quantum theory for spin-changing transitions is developed and applied to calculate the spin exchange and spin relaxation rates of Li and K atoms in cryogenic 3He^{3}\mathrm{He}3He gas. Magnetic trapping experiments provide upper bounds to the spin exchange rates for $\mathrm{Li}\text{\ensuremath{-}}^{3}\mathrm{He}$ and $\mathrm{K}\text{\ensuremath{-}}^{3}\mathrm{He}$, which are in agreement with the present theory. Our calculations demonstrate that the alkali-metal atoms have extremely slow spin depolarization rates, suggesting a number of potential applications in precision spectroscopy and quantum optics.
The van der Waals coefficients for the alkali-metal atoms from Na to Fr interacting in their ground states are calculated using relativistic ab initio methods. The accuracy of the calculations is estimated by also evaluating atomic static electric-dipole polarizabilities and coefficients for the interaction of the atoms with a perfectly conducting wall. The results are in excellent agreement with the latest data from studies of magnetic field induced Feshbach resonances in ultracold collisions of Na and of Rb atoms. For Cs we provide critically needed data for ultracold collision studies.
Collisions of alkali-metal atoms in the ground state with the electron spin S = 1/2 are accompanied by exchange of electron coordinates between colliding particles, which leads to polarization transfer between them (i.e., to the well-known phenomenon of spin exchange). In addition, along with the polarization transfer from one partner to another, the magnetic resonance lines of colliding atoms are broadened and shifted in spin-exchange collisions. In particular the last two processes depend on the complex spin-exchange cross section. The real part of the cross section determines the so-called "spin-exchange cross section," which is responsible for the broadening of magnetic resonance lines, while the imaginary part determines the shift cross section, which governs the frequency shift of magnetic resonance. In order to describe the spin-exchange process one have to know complex spin-exchange cross sections. Complex spin-exchange cross sections are calculated on the basis of the data on the singlet (X 1 Σ + ) and triplet (a 3 Σ + ) potentials describing the interaction alkali-metal atoms in the ground state. Collisions of alkali-metal atoms Cs, Rb, K, Na in the ground state are considered in the energy interval of 10 −4 −10 −2 au.
The interaction of alkali K and Rb atoms that reside in the ground state is considered in the range of collision energies E = 10−4 to 10−2 au. The singlet (X 1Σ+) and triplet (a 3Σ+) interaction potentials available in the literature are analyzed and modified. For the KRb dimer in the range of interatomic distances 15–21a 0, we chose analytical representations of the singlet and triplet potentials that more accurately describe the interaction of alkali Rb and K atoms in the ground state. Complex cross sections of the spin exchange are calculated for the first time that permit one to calculate the processes of polarization transfer and relaxation times, as well as shifts in the magnetic resonance frequencies caused by K-Rb spin exchange collisions.
We present a comprehensive theory of nuclear spin polarization of 3He{}^{3}\mathrm{He}3He and 129Xe{}^{129}\mathrm{Xe}129Xe gases by spin-exchange collisions with optically pumped alkali-metal vapors. The most important physical processes considered are (1) spin-conserving spin-exchange collisions between like or unlike alkali-metal atoms; (2) spin-destroying collisions of the alkali-metal atoms with each other and with buffer-gas atoms; (3) electron-nuclear spin-exchange collisions between alkali-metal atoms and 3He{}^{3}\mathrm{He}3He or 129Xe{}^{129}\mathrm{Xe}129Xe atoms; (4) spin interactions in van der Waals molecules consisting of a Xe atom bound to an alkali-metal atom; (5) optical pumping by laser photons; (6) spatial diffusion. The static magnetic field is assumed to be small enough that the nuclear spin of the alkali-metal atom is well coupled to the electron spin and the total spin is very nearly a good quantum number. Conditions appropriate for the production of large quantities of spin-polarized 3He{}^{3}\mathrm{He}3He or 129Xe{}^{129}\mathrm{Xe}129Xe gas are assumed, namely, atmospheres of gas pressure and nearly complete quenching of the optically excited alkali-metal atoms by collisions with N2{\mathrm{N}}_{2}N2​ or H2{\mathrm{H}}_{2}H2​ gas. Some of the more important results of this work are as follows: (1) Most of the pumping and relaxation processes are sudden with respect to the nuclear polarization. Consequently, the steady-state population distribution of alkali-metal atoms is well described by a spin temperature, whether the rate of spin-exchange collisions between alkali-metal atoms is large or small compared to the optical pumping rate or the collisional spin-relaxation rates. (2) The population distributions that characterize the response to sudden changes in the intensity of the pumping light are not described by a spin temperature, except in the limit of very rapid spin exchange. (3) Expressions given for the radio-frequency (rf) resonance linewidths and areas can be used to make reliable estimates of the local spin polarization of the alkali-metal atoms. (4) Diffusion effects for these high-pressure conditions are mainly limited to thin layers at the cell surface and at internal resonant surfaces generated by radio-frequency magnetic fields when the static magnetic field has substantial spatial inhomogeneities. The highly localized effects of diffusion at these surfaces are described with closed-form analytic functions instead of the spatial eigenmode expansions that are appropriate for lower-pressure cells.