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arXiv:1302.6894 · Physical Review A

Spin-velocity correlations of optically pumped atoms

R. Marsland, B. H. McGuyer, Ben A. Olsen, W. Happer

Published Aug 3, 2012• 6 citations
arXivHTMLPDF

Abstract

We present efficient theoretical tools for describing the optical pumping of atoms by light propagating at arbitrary directions with respect to an external magnetic field, at buffer-gas pressures that are small enough for velocity-selective optical pumping (VSOP) but large enough to cause substantial collisional relaxation of the velocities and the spin. These are the conditions for the sodium atoms at an altitude of about 100 km that are used as guidestars for adaptive optics in modern ground-based telescopes to correct for aberrations due to atmospheric turbulence. We use spin and velocity relaxation modes to describe the distribution of atoms in spin space (including both populations and coherences) and velocity space. Cusp kernels are used to describe velocity-changing collisions. Optical pumping operators are represented as a sum of poles in the complex velocity plane. Signals simulated with these methods are in excellent agreement with previous experiments and with preliminary experiments in our laboratory.

DOI
10.1103/physreva.86.023404

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We present efficient theoretical tools for describing the optical pumping of atoms by light propagating at arbitrary directions with respect to an external magnetic field, at buffer-gas pressures that are small enough for velocity-selective optical pumping (VSOP) but large enough to cause substantial collisional relaxation of the velocities and the spin. These are the conditions for the sodium atoms at an altitude of about 100 km that are used as guidestars for adaptive optics in modern ground-based telescopes to correct for aberrations due to atmospheric turbulence. We use spin and velocity relaxation modes to describe the distribution of atoms in spin space (including both populations and coherences) and velocity space. Cusp kernels are used to describe velocity-changing collisions. Optical pumping operators are represented as a sum of poles in the complex velocity plane. Signals simulated with these methods are in excellent agreement with previous experiments and with preliminary experiments in our laboratory.
We experimentally demonstrate how magnetic depolarization of velocity-selective optical pumping can be used to single out the collisional cusp kernel best describing spin- and velocity-relaxing collisions between potassium atoms and low-pressure helium. The range of pressures and transverse fields used simulate the optical pumping regime pertinent to sodium guidestars employed in adaptive optics. We measure the precession of spin-velocity modes under the application of transverse magnetic fields, simulating the natural configuration of mesospheric sodium optical pumping in the geomagnetic field. We also provide a full theoretical account of the experimental data using the recently developed cusp kernels, which realistically quantify velocity damping collisions in this optical pumping regime. A single cusp kernel with a sharpness $s=13\ifmmode\pm\else\textpm\fi{}2$ provides a global fit to the K-He data.
We discuss optical pumping when (a) the collision rates of optically pumped atoms with atoms or molecules of the background gas are small enough that individual velocity groups can be preferentially excited by a monochromatic light beam, (b) the collision rates are still fast enough to partially transfer the spin polarization to other velocity groups, and (c) there are nonnegligible losses of polarization due to collisional spin relaxation and Larmor precession. These conditions lead to a strong correlation between the velocity and the spin polarization of the atoms---that is, to ``spin-tagging'' of the different velocity groups. This regime is similar to that of optically pumped 23Na^{23}\mathrm{Na}23Na atoms of the Earth's upper atmosphere, but it is seldom encountered in laboratory experiments. For cooling and trapping experiments, the collision rates with background gas are negligible. For gas-cell experiments the velocity-changing rates are normally so fast compared to spin relaxation or Larmor precession rates that the atoms have a Maxwellian velocity distribution with negligible correlation between the spin polarization and the velocity. We analyze the limiting cases of strong and weak collisions, which change the velocity by a large or small fraction, respectively, of the mean thermal velocity. The Keilson-Storer model [J. Keilson and A. E. Storer, Q. Appl. Math. 10, 243 (1952)] is used to discuss strong collisions, with memory parameter $\ensuremath{\alpha}=0$ and weak collisions with $\ensuremath{\alpha}\ensuremath{\rightarrow}1$. For weak collisions, the physics can be modeled by coupled Fokker-Planck equations, identical to those for forced diffusion in a harmonic-oscillator potential well. In this limit there are solutions analogous to the quantum mechanical coherent states of a harmonic oscillator.
Optical pumping performed with a quasi monochromatic laser beam in an atomic gas introduces a redistribution of Zeeman populations selectively in a single velocity class. In the limit of low pumping intensity the rate theory is valid for a description of velocity-selective optical pumping (V.S.O.P.). Well-defined atomic observables (population, orientation, alignment) and their velocity-correlated collisional relaxation can be studied. Also, a modified scheme for the detection of second order effects of optical pumping allows one to observe light shift induced signals. In particular, V.S.O.P. and its combination with modulated pumping, magnetic depolarization (level crossing), and magnetic resonance techniques provide information about the atomic collision characteristics such as collision rates and kernels for velocity-changing collisions.
We report on a quantitative experimental investigation of velocity-changing collisions by means of velocity-selective optical pumping (VSOP). We have calculated the VSOP line shape for an atom with hyperfine structure with the use of two phenomenological kernels for the collision effects: the Keilson-Storer kernel, and a two-term kernel consisting of a broad Keilson-Storer part and a narrower Gaussian component. Corrections were included to account for the finite absorption in the sample and the backward reflection of the pumping beam. The experiments were carried out in sodium vapor with neon as the perturber gas. The D1{D}_{1}D1​ line of sodium was used for optical pumping, and the orientation of the ground state was detected. Free parameters of the theory were determined by fitting the predicted line shapes to experimental curves. The Keilson-Storer kernel proved unsatisfactory, but the two-term kernel reproduced well the observed line shapes over the entire collision profiles in the neon pressure range 0-57 mtorr. In an independent experiment using rapidly modulated VSOP we also measured directly the cross section of velocity-changing collisions: $\ensuremath{\sigma}=(1.13\ifmmode\pm\else\textpm\fi{}0.10)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}$ cm2{\mathrm{cm}}^{2}cm2. The large weight obtained for the narrow Gaussian from the fits, as well as the collision cross section which is three times as large as the cross section deduced from tabulated gas kinetic radii, may indicate the presence of collisions with relatively small velocity changes in addition to hard-sphere encounters.
Optical pumping is fundamental to high-precision measurement using thermal alkali-metal atoms in vapor cells. In applications such as atomic magnetometry, buffer gases (e.g., N2\mathrm{N}_2N2​ or He\mathrm{He}He) at specific pressures are introduced to quench fluorescence and mitigate wall relaxation. In the high-pressure limit (e.g., the N2\mathrm{N}_2N2​ pressure pN2>1p_{\mathrm{N}_2}> 1pN2​​>1~atm), where collisional broadening exceeds hyperfine splittings of the atoms, optical pumping theory provides a clear description of the angular momentum exchange between photons and atomic spins. However, in many magnetic sensing scenarios, the high-pressure approximation becomes inadequate as its pressure conditions are not strictly satisfied. Consequently, an explicit description of optical pumping under realistic pressures is critical for selecting operating points and enhancing system performance. To address this, we develop a unified theoretical framework of optical pumping in the quasi-high-pressure regime, where collisional broadening is comparable to the ground-state hyperfine splitting. We demonstrate that light absorption, spin polarization, and magnetic-resonance linewidth in this regime differ significantly from those predicted by the high-pressure limit and offer favorable operating conditions. Our study extends conventional modeling and offers critical guidance for atomic magnetometry operating under realistic buffer gas pressures.
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.