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International Conference Laser Optics (ICLO)

Influence of inelastic collisions on the efficiency of optical pumping of alkali atoms in a gas cell

К. А. Баранцев, A.N. Litvinov

Published Jun 20, 2022• 0 citations
Publisher

Abstract

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.

DOI
10.1109/iclo54117.2022.9840098

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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.
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.
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.
The optical orientation of the angular momenta of alkali atoms in the presence of a buffer gas (molecular nitrogen) has been studied experimentally. It has been shown that, even at a low concentration of molecular nitrogen in the cell, the excitation of 133 Cs atoms from the lower hyperfine level with F = 3, which belongs to the ground 2 S 1/2 state, results in a larger amplitude of the magnetic resonance than the excitation from the hyperfine level with F = 4. This result has been theoretically explained under the assumption that the spin state of the alkali atomic nucleus does not change at collision with a nitrogen molecule, which is accompanied by a nonradiative transition of the alkali atom from the excited 2 P 1/2 state to the ground 2 S 1/2 state.
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 relaxation and generation of multipole orientations in a heavy-alkali-metal vapor in the presence of a weak static magnetic field are theoretically studied both for populations and for Zeeman coherences by taking into account the effects on the evolution of the atomic density matrix of the relaxation processes (by alkali-atom--buffer-gas, alkali-atom--alkali-atom with spin exchange and alkali-atom--cell-wall collisions) and of the optical pumping with any light polarization and spectral distribution. The dependence of the stationary-state multipole orientations on the pumping characteristic parameters is numerically analyzed. The detection process of these orientations is also studied.
Optically Pumped Magnetometers use light to drive an atomic vapor into a Non-Equilibrium Steady State for sensing. This kind of state is achieved when spin-exchange collisions, together with optical pumping, dominate the relaxation dynamics, redistributing the atomic populations and thereby shaping the steady-state configuration. Despite the rapid advancement of atomic magnetometer technology, a comprehensive thermodynamic analysis of the state preparation is largely unexplored. We apply a thermodynamic framework to alkali atoms in a vapor cell, modeling their interactions with the pump laser and their relaxation via spin-exchange and spin-destruction collisions. We analyze how the pump rate and light polarization determine the non-equilibrium steady state, quantifying irreversibility via entropy production, assessing useful energy via ergotropy, and defining the spin-polarization efficiency. Finally, we establish a connection between metrological performance and the Quantum Fisher Information (QFI), demonstrating that a higher thermodynamic efficiency directly translates into an improved fundamental bound on magnetometer sensitivity. These results provide insights for optimizing state preparation in quantum sensors.