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Physical Review A

Effect of rapid spin exchange on the magnetic-resonance spectrum of alkali vapors

W. Happer, A. C. Tam

Published Nov 1, 1977• 292 citations
Publisher

Abstract

It was recently discovered that when there are sufficiently rapid spin-exchange collisions in an alkali-metal vapor, the rf magnetic-resonance frequency of the ground-state atoms becomes a constant fractional value (e.g., $\frac{4}{11}$ for Cs) of the Larmor frequency, and the linewidth becomes inversely proportional to the spin-exchange rate. These properties are in complete contrast to those in the slow spin-exchange limit. We present a theoretical analysis of these properties, and we predict some additional new effects for rapid spin exchange. Four theories are presented; an intuitive-vector model, a perturbation treatment, numerical solutions of complex non-Hermitian matrices, and a statistical analysis of the effect of rapid transfers between two Zeeman multiplets. These theories all provide, to varying degrees, consistent quantitative answers to the problem of how spin exchange affects magnetic resonance in an alkali vapor.

DOI
10.1103/physreva.16.1877

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Spin-exchange frequency shift in alkali-metal-vapor cell frequency standards

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In this paper we calculate the effect of spin-exchange collisions in alkali-metal vapors. In the framework of the high-energy approximation, we evaluate the spin-exchange cross sections related to the line broadening and to the frequency shift of the ground state hyperfine transition. We do the calculation for the four isotopes, $^{23}\mathrm{Na}$, $^{39}\mathrm{K}$, $^{87}\mathrm{Rb}$, and $^{133}\mathrm{Cs}$. The results are used in particular to evaluate the spin-exchange frequency shift in Rb vapor cell frequency standards used in many applications. It turns out that, due to possible fluctuations in the atomic density, spin exchange may affect significantly the medium and long term frequency stability of the frequency standard.

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We present a comprehensive theory of nuclear spin polarization of ${}^{3}\mathrm{He}$ and ${}^{129}\mathrm{Xe}$ 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 ${}^{3}\mathrm{He}$ or ${}^{129}\mathrm{Xe}$ 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 ${}^{3}\mathrm{He}$ or ${}^{129}\mathrm{Xe}$ gas are assumed, namely, atmospheres of gas pressure and nearly complete quenching of the optically excited alkali-metal atoms by collisions with ${\mathrm{N}}_{2}$ or ${\mathrm{H}}_{2}$ 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.

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Magnetic-resonance-frequency shifts in spin-exchange collisions of Rb and Cs alkali-metal atoms

Victor A. Kartoshkin

On the basis of data on spin-exchange complex cross sections in the Rb–Rb and Cs–Rb systems, the magnetic-resonance-frequency shifts of rubidium atoms upon collisions in a mixture of Cs–Rb alkalimetal atoms are calculated. The results obtained are compared with the experimental data and the previous theoretical data.

Optics and Spectroscopy•Sep 1, 2017•1 citation
It was recently discovered that when there are sufficiently rapid spin-exchange collisions in an alkali-metal vapor, the rf magnetic-resonance frequency of the ground-state atoms becomes a constant fractional value (e.g., 411\frac{4}{11}114​ for Cs) of the Larmor frequency, and the linewidth becomes inversely proportional to the spin-exchange rate. These properties are in complete contrast to those in the slow spin-exchange limit. We present a theoretical analysis of these properties, and we predict some additional new effects for rapid spin exchange. Four theories are presented; an intuitive-vector model, a perturbation treatment, numerical solutions of complex non-Hermitian matrices, and a statistical analysis of the effect of rapid transfers between two Zeeman multiplets. These theories all provide, to varying degrees, consistent quantitative answers to the problem of how spin exchange affects magnetic resonance in an alkali vapor.
Spin-exchange collisions often play a dominant role in the broadening of Zeeman resonances in an alkali-metal vapor. Contrary to intuitive expectations, at high alkali-metal densities this broadening can be completely eliminated by operating in a low magnetic field, allowing construction of ultrasensitive atomic magnetometers. We describe a detailed study of the Zeeman resonance frequencies and linewidths as a function of the magnetic field, alkali-metal density, and the degree of spin polarization of the atoms. Due to the nonlinear nature of the density matrix equations describing the spin-exchange collisions both the gyromagnetic ratio and the linewidth change as a function of the polarization. The results of experimental measurements are in excellent agreement with analytical and numerical solutions of the density matrix equations.
The study of magnetic-resonance linewidth is crucial in magnetic-resonance physics and its applications. Previous studies focused on the linewidth of alkali metal atoms within the spin-exchange relaxation-free regime near zero magnetic field and in strong magnetic fields where Zeeman resonances are well resolved due to the quadratic Zeeman effect. However, the linewidth in the unresolved-Zeeman-resonance regime, which is prevalent in various magnetometer and comagnetometer applications, is not well understood. To address this, we developed a theoretical framework based on the master equation for alkali metal atoms and solved it under the rotating-wave approximation and weak-driving conditions. Our numerical calculations and analytical expressions reveal that the light-narrowing effect occurs only when the ratio of the spin-exchange rate to the spin destruction rate exceeds a critical value. Additionally, we show that the linewidth in the unresolved Zeeman-resonance regime is significantly influenced by the mutual coupling of quantum coherence between different Zeeman sublevels. These findings provide a theoretical tool for understanding spin relaxation in alkali-metal atoms and optimizing the performance of atomic magnetometers and comagnetometers operating in this regime.
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.
In this paper we calculate the effect of spin-exchange collisions in alkali-metal vapors. In the framework of the high-energy approximation, we evaluate the spin-exchange cross sections related to the line broadening and to the frequency shift of the ground state hyperfine transition. We do the calculation for the four isotopes, 23Na^{23}\mathrm{Na}23Na, 39K^{39}\mathrm{K}39K, 87Rb^{87}\mathrm{Rb}87Rb, and 133Cs^{133}\mathrm{Cs}133Cs. The results are used in particular to evaluate the spin-exchange frequency shift in Rb vapor cell frequency standards used in many applications. It turns out that, due to possible fluctuations in the atomic density, spin exchange may affect significantly the medium and long term frequency stability of the frequency standard.
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.