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Physical Review

Spin Relaxation and Line Width in Alkali Metal Vapors

Arnold L. Bloom

Published May 1, 1960• 12 citations
Publisher

Abstract

Relaxation constants ${T}_{1}$ and ${T}_{2}$ have been computed for experiments involving optical pumping and optical detection in alkali metal vapor. The calculations have been performed for several possible spin relaxation mechanisms; namely, magnetic dipole, electric quadrupole, spin exchange, and the optical pumping process itself. For all of these mechanisms a reorientation experiment will approximately predict a spin resonance line width (equivalent to the statement ${T}_{1}\ensuremath{\approx}{T}_{2}$ for spin-\textonehalf{} particles.) However, a spin reorientation experiment of the type originally performed by Dehmelt, employing circularly polarized light, gives approximate results because of the nonexponential character of the reorientation. A more suitable experiment is one employing hyperfine population differences and unpolarized light.

DOI
10.1103/physrev.118.664

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NEW STUDIES OF OPTICAL PUMPING, SPIN RESONANCES, AND SPIN EXCHANGE IN MIXTURES OF INERT GASES AND ALKALI-METAL VAPORS

Yuan‐Yu Jau

In this thesis, we present new studies of alkali-hyperfine resonances, new optical pumping of alkali-metal atoms, and the new measurements of binary spin-exchange cross-section between alkali-metal atoms and xenon atoms. We report a large light narrowing effect of the hyperfine end-resonance signals, which was predicted from our theory and observed in our experiments. By increasing the intensity of the circularly polarized pumping beam, alkali-metal atoms are optically pumped into a state of static polarization, and trapped into the hyperfine end-state. Spin exchange between alkali-metal atoms has minimal effect on the end-resonance of the highly spinpolarized atoms. This new result will possibly benefit the design of atomic clocks and magnetometer. We also studied the pressure dependence of the atomic-clock resonance linewidth and pointed out that the linewidth was overestimated by people in the community of atomic clock. Next, we present a series study of coherent population trapping (CPT), which is a promising technique with the same or better performance compared to the traditional microwave spectroscopy. For miniature atomic clocks, CPT method is thought to be particularly advantages. From our studies, we invented a new optical-pumping method, push-pull optical pumping, which can pump atoms into nearly pure 0-0 superposition state, the superposition state of the two ground-state hyperfine sublevels with azimuthal quantum number m = 0. We believe this new invention will bring a big advantage to CPT frequency standards, the quantum state preparation for cold atoms or hot vapor, etc. We also investigated the pressure dependence of CPT excitation and the line shape of the CPT resonance theo-

•Jan 1, 2005•3 citations
Relaxation constants T1{T}_{1}T1​ and T2{T}_{2}T2​ have been computed for experiments involving optical pumping and optical detection in alkali metal vapor. The calculations have been performed for several possible spin relaxation mechanisms; namely, magnetic dipole, electric quadrupole, spin exchange, and the optical pumping process itself. For all of these mechanisms a reorientation experiment will approximately predict a spin resonance line width (equivalent to the statement T1\ensuremath≈T2{T}_{1}\ensuremath{\approx}{T}_{2}T1​\ensuremath≈T2​ for spin-\textonehalf{} particles.) However, a spin reorientation experiment of the type originally performed by Dehmelt, employing circularly polarized light, gives approximate results because of the nonexponential character of the reorientation. A more suitable experiment is one employing hyperfine population differences and unpolarized light.
A variation of the usual method of atomic orientation of alkali metal vapors by optical pumping is proposed. This variation consists of employing a single circularly polarized D1{D}_{1}D1​ line as pumping radiation, instead of a mixture of the two DDD lines. Under these conditions, one magnetic substate of the ground state is transparent to the pumping radiation. It is shown that for a sufficiently intense light source and relatively weak relaxation, the entire population of the vapor will tend to be pumped into this single state, resulting in nearly one-hundred percent atomic orientation. The pumping process is analyzed in detail for sodium vapor illuminated with $3{P}_{\frac{1}{2}}\ensuremath{-}3{S}_{\frac{1}{2}}$ radiation, and the time dependence of the populations of the eight magnetic sublevels of the ground state is computed. It is shown that in the steady state, the light absorption by the vapor is linear rather than exponential with distance. A simple method of measuring relaxation times based on this observation is suggested. The conditions under which the imprisonment of resonance radiation limits the size of the oriented sample are discussed, and it is suggested that the proposed technique will allow the alignment of larger samples than is possible by the usual method of optical pumping.
A vapor of paramagnetic atoms, under conditions in which electronic spin exchange takes place faster than collisional spin relaxation, should acquire a spontaneous spin polarization when illuminated by unpolarized light tuned to excite only certain ground-state atomic hyperfine levels. In magnetic fields above a certain size, the atomic polarization has two stable states, either parallel or antiparallel to the field. Experiments to demonstrate this effect and explore possible applications may be feasible by the use of alkali-metal vapors.
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.
Rate equations for the optical pumping of alkali-metal vapors simultaneously subject to pumping, relaxation in the excited state, and relaxation in the ground state are shown to yield analytic solutions for the alkali-metal electronic and nuclear-spin polarizations in the limit of weak pumping. Nuclear-spin and hyperfine-interaction effects are properly included. Analysis of the double-exponential form of the pumping transient of the ground-state electronic-spin polarization is shown to yield new methods for the measurement of cross sections for collisional relaxation in both the ground and excited states. Formulas are derived that relate relaxation cross sections to experimentally measurable parameters. Formulas describing the influence of nuclear spin on signals obtained from standard depolarization of resonance-radiation experiments also are provided. Ambiguities in earlier optical-pumping experiments and calculations arising from oversimplified descriptions of relaxation processes are discussed.
A generalized model for the magnetic resonance signal corresponding to the 0-0 hyperfine transition in an optically pumped alkali-metal vapor is presented. Under conditions of microwave power broadening, the model predicts ``anomalous'' light broadening and ``anomalous'' relaxation narrowing of the magnetic resonance linewidth. Good agreement between theory and experiment was obtained in an experiment that confirmed the prediction of anomalous light broadening. These results show that the 0-0 hyperfine transition cannot be described as a simple two-level system; rather, the alkali-atom's nuclear spin plays an important role in determining the magnetic resonance linewidth.
In this thesis, we present new studies of alkali-hyperfine resonances, new optical pumping of alkali-metal atoms, and the new measurements of binary spin-exchange cross-section between alkali-metal atoms and xenon atoms. We report a large light narrowing effect of the hyperfine end-resonance signals, which was predicted from our theory and observed in our experiments. By increasing the intensity of the circularly polarized pumping beam, alkali-metal atoms are optically pumped into a state of static polarization, and trapped into the hyperfine end-state. Spin exchange between alkali-metal atoms has minimal effect on the end-resonance of the highly spinpolarized atoms. This new result will possibly benefit the design of atomic clocks and magnetometer. We also studied the pressure dependence of the atomic-clock resonance linewidth and pointed out that the linewidth was overestimated by people in the community of atomic clock. Next, we present a series study of coherent population trapping (CPT), which is a promising technique with the same or better performance compared to the traditional microwave spectroscopy. For miniature atomic clocks, CPT method is thought to be particularly advantages. From our studies, we invented a new optical-pumping method, push-pull optical pumping, which can pump atoms into nearly pure 0-0 superposition state, the superposition state of the two ground-state hyperfine sublevels with azimuthal quantum number m = 0. We believe this new invention will bring a big advantage to CPT frequency standards, the quantum state preparation for cold atoms or hot vapor, etc. We also investigated the pressure dependence of CPT excitation and the line shape of the CPT resonance theo-