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Journal of Experimental and Theoretical Physics

Counterpolarization of an Ensemble of Alkaline Atoms during Optical Pumping: Study with Allowance for Atomic Motion

К. А. Баранцев, A. N. Litvinov, Anatoly S. Pazgalev, Anton K. Vershovskii

Published Feb 1, 2021• 3 citations
Publisher

Abstract

Abstract A theory is developed for the optical pumping of alkali atoms with allowance for Zeeman and hyperfine structures and atomic motion in the model of instantaneous mixing between the Zeeman and hyperfine sublevels in an excited state. The appearance of the angular momentum in the 87Rb and 133Cs atoms that is opposite to the momentum of the photons pumping these atoms is studied. This effect is found to be most pronounced in the D2 line. The influence of the buffer gas pressure and the optical pumping intensity on the features of this effect is analyzed. The influence of the counterpolarization effect on the parameters of high-sensitivity quantum magnetometers is discussed.

DOI
10.1134/s106377612101009x

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Abstract A theory is developed for the optical pumping of alkali atoms with allowance for Zeeman and hyperfine structures and atomic motion in the model of instantaneous mixing between the Zeeman and hyperfine sublevels in an excited state. The appearance of the angular momentum in the 87Rb and 133Cs atoms that is opposite to the momentum of the photons pumping these atoms is studied. This effect is found to be most pronounced in the D2 line. The influence of the buffer gas pressure and the optical pumping intensity on the features of this effect is analyzed. The influence of the counterpolarization effect on the parameters of high-sensitivity quantum magnetometers is discussed.
Abstract We analyze the polarization of the total angular momentum of alkali atoms in a gas cell with a buffer gas under pumping by monofrequency circularly polarized laser radiation. The mathematical model takes into account the motion of atoms and collisions preserving the nuclear spin under the chaotization of the angular momentum of the outer electron shell, total hyperfine structure, and the Zeeman structure. We analyze the stationary solution to equations for the density matrix of alkali atoms and the effect produced on them by the fraction of inelastic collision in which the quenching of atomic excitation takes place. We consider the contribution of various hyperfine states to the polarization of alkali atoms. The results are compared with the results of the model of instantaneous mixing of populations in the excited state.
Using a three-level model and semiclassical density matrix formalism, we show that optical pumping influences both line positions and amplitudes in Doppler-broadened alkali-atom D1 and D2 spectra for intensities much lower than the two-level atom saturation intensity. The influence on the D2 spectrum is particularly interesting due to the presence of closed hyperfine transitions unaffected by optical pumping. This effect is of importance for example when lasers are frequency stabilized using linear absorption or when the alkali-atom vapour pressure is determined using absorption measurements.
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.
The effect of excited-state mixing on the optical pumping of alkali-metal vapors is considered for the case where the energy separation between the 2P12^{2}P_{\frac{1}{2}}2P21​​ and 2P32^{2}P_{\frac{3}{2}}2P23​​ first excited states is relatively large, allowing the isolation of mixing effects within a particular JJJ level. Two models for the mixing process are proposed, one a random reorientation of the total electronic angular momentum J, and the other a reorientation of J subject to the selection rule $\ensuremath{\Delta}{m}_{J}=0, \ifmmode\pm\else\textpm\fi{}2$. The probabilities for mixing transitions among JJJ-state sublevels have been calculated for an alkali atom of nuclear spin 32\frac{3}{2}23​, and can be used to calculate the optical-pumping transition probabilities for a vapor subject to any degree of excited-state mixing. Several possible experiments suggested by these calculations are discussed.
We study the processes of optical pumping of alkali metal atoms in the gas cell with buffer gas for the quantum magnetometers. The value of pumped magnetic moment is strongly influenced by the collision effects. Collisions of alkali atoms with the buffer gas lead to partial destruction of the atomic quantum state. As a first approximation, we can assume that the state of electronic shell collapses, but the state of the nucleus is saved. This work is devoted to the description of this effect and its impact to the polarization of the magnetic moment.
In the optical excitation of atoms with polarized light, producing excited atoms, only some of the Zeeman sublevels of the excited state are actually reached, so that large differences of population can be built up between Zeeman sublevels or between hyperfine structure (hfs) levels. This property can be used to detect radio-frequency resonance in optically excited atomic states. These resonances produce a characteristic change in intensity or in the degree of polarization of the light re-emitted. Zeeman intervals, Stark effects, and hfs intervals can be measured in this manner. (The Stark constant of the 63P1 level of Hg and the electric quadrupole moments of the alkali atoms have been obtained in this way.)The technique of “optical pumping” gives a way to concentrate atoms in some of the Zeeman sublevels of one of the hfs levels of the ground state.Atomic orientation has been obtained with the Na atom, in an atomic beam and in the vapor in equilibrium with the metal. The orientation effects have been studied by detection of radio-frequency resonance signals in the ground state. Orientation can be increased many times by adding a variable pressure of a foreign gas to the pure Na vapor. Because of the coupling between nuclear spin and electron spin, nuclear orientation is produced at the same time as atomic orientation.