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arXiv:2305.11500 · Physical Review A

Wall-collision effect on optically polarized atoms in small and hot vapor cells

Yue Chang, Jie Qin

Published Feb 16, 2024• 7 citations
arXivHTMLPDF

Abstract

In atomic vapor cells, atoms collide with the inner surface, causing their spin to randomize on the walls. This wall-depolarizing effect can be diffusive and it becomes more pronounced in smaller vapor cells under high temperatures. In this work we investigate the polarization of optically pumped alkali-metal atoms in a millimeter-sized cell heated to $150{\phantom{\rule{0.16em}{0ex}}}^{\ensuremath{\circ}}\text{C}$. We consider two extreme boundary conditions, fully depolarizing and nondepolarizing boundaries, and we provide an analytical estimation of the polarization difference between them. In the nondepolarizing case, the pump beam's absorption is proportional to the average atomic polarization. However, for fully depolarizing walls, the absorption peak may correspond to a polarization minimum. To mitigate the wall effect, we propose reducing the pump beam's diameter while maintaining the pump power to prevent illumination of the cell wall and increase the pump intensity in the central area. This is crucial for compact vapor-cell devices where the laser frequency cannot be detuned since it is locked to the absorption peaks. Additionally, we analyze the wall-depolarizing effect on the performance of an alkali-metal atomic magnetometer operating in the spin-exchange relaxation-free regime. We show that the signal strength is highly limited by wall collisions and we provide an upper bound for it.

DOI
10.1103/physreva.109.023113

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In atomic vapor cells, atoms collide with the inner surface, causing their spin to randomize on the walls. This wall-depolarizing effect can be diffusive and it becomes more pronounced in smaller vapor cells under high temperatures. In this work we investigate the polarization of optically pumped alkali-metal atoms in a millimeter-sized cell heated to 150\ensuremath∘C150{\phantom{\rule{0.16em}{0ex}}}^{\ensuremath{\circ}}\text{C}150\ensuremath∘C. We consider two extreme boundary conditions, fully depolarizing and nondepolarizing boundaries, and we provide an analytical estimation of the polarization difference between them. In the nondepolarizing case, the pump beam's absorption is proportional to the average atomic polarization. However, for fully depolarizing walls, the absorption peak may correspond to a polarization minimum. To mitigate the wall effect, we propose reducing the pump beam's diameter while maintaining the pump power to prevent illumination of the cell wall and increase the pump intensity in the central area. This is crucial for compact vapor-cell devices where the laser frequency cannot be detuned since it is locked to the absorption peaks. Additionally, we analyze the wall-depolarizing effect on the performance of an alkali-metal atomic magnetometer operating in the spin-exchange relaxation-free regime. We show that the signal strength is highly limited by wall collisions and we provide an upper bound for it.
We have experimentally and theoretically investigate the effect of optical pump beam size on narrowband spin polarized optical pumping of alkali atom vapor. We developed a six-level model describing narrowband spin polarized optical pumping of alkali atoms and applied this model to an atomic vapor cell, accounting for atomic transit time through the optical beam and wall collision effects. Our expression for the wall collision effects is derived from the diffusion model. Overall, we obtained good agreement between theory and experimentally measured relaxation time constants.
Field-inhomogeneity-induced relaxation of atomic spins confined in vapor cells with depolarizing walls is studied. In contrast to nuclear spins, such as noble-gas spins, which experience minimal polarization loss at cell walls, atomic spins in uncoated cells undergo randomization at the boundaries. This distinct boundary condition results in a varied dependence of the relaxation rate on the field gradient. By solving the Bloch-Torrey equation under fully depolarizing boundary conditions, we illustrate that the relaxation rate induced by field inhomogeneity is more pronounced for spins with a smaller original relaxation rate (in the absence of the inhomogeneous field). We establish an upper limit for the relaxation rate through calculations in the perturbation regime. Moreover, we connect it to the spin-exchange-relaxation-free magnetometers, demonstrating that its linewidth is most sensitive to inhomogeneous fields along the magnetometer's sensitive axis. Our theoretical result agrees with the experimental data for cells subjected to small pump power. A deviation in high input-power scenarios arises from pump field attenuation, resulting in a nonuniformly distributed light shift that behaves like an inhomogeneous magnetic field.
Spatial distribution of the polarization in Rb vapor optically pumped with 21 Ne has been modeled numerically with 40 mW laser beam power, 180°C cell temperature, 1 bar cell pressure, and 6 mm × 15 mm pancake-cell geometry. An inhomogeneity of polarization throughout the cell results from a wall relaxation of polarized media and a decay of the pumping beam. For small cells characteristic of experimental conditions, a contribution of wall relaxation to the total alkali relaxation rate can become significant, demanding more accurate evaluation than afforded by analytical model based on average parameters.
Abstract The spin polarization and spatial homogeneity of alkali metal atoms are critical characteristics that determine the performance of spin-exchange relaxation-free magnetometers. In buffer gas cells, these characteristics are influenced by optical broadening and alkali atomic motional restriction imposed by the buffer gas. In coated cells, the protective effect of the coating on atomic spins, combined with rapid atomic diffusion, leads to significantly superior spin polarization characteristics compared to those in high-pressure buffer gas cells. However, due to neglecting the influence of atom-coating interactions on atomic motion, the existing spin polarization and spatial distribution models fail to accurately describe the polarization characteristics in coated cells. In this paper, based on the Langevin–Bloch equation, a dynamic model considering interaction effects between alkali metal atoms and the coating as well as between the pump light and the hyperfine levels of alkali metal atoms is proposed to accurately describe the spin polarization and spatial distribution in coated cells. To validate the proposed model, a series of experiments were carried out. The results demonstrate that coated cells can maintain high spin polarization and spatial homogeneity even under conditions of low pump intensity and high temperature, which are in good agreement with the simulations. This work provides a theoretical reference for the design of high-performance and low-power quantum sensors.
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.
Antirelaxation surface coatings allow long spin relaxation times in alkali-metal cells without buffer gas, enabling faster diffusion of the alkali atoms throughout the cell and giving larger signals due to narrower optical linewidths. Effective coatings were previously unavailable for operation at temperatures above 80 °C. We demonstrate that octadecyltrichlorosilane (OTS) can allow potassium or rubidium atoms to experience hundreds of collisions with the cell surface before depolarizing, and that an OTS coating remains effective up to about 170 °C for both potassium and rubidium. We consider the experimental concerns of operating without buffer gas and with minimal quenching gas at high vapor density, studying the stricter need for effective quenching of excited atoms and deriving the optical rotation signal shape for atoms with resolved hyperfine structure in the spin-temperature regime. As an example of a high-temperature application of antirelaxation coated alkali vapor cells, we operate a spin-exchange relaxation-free atomic magnetometer with sensitivity of 6 fT/Hz and magnetic linewidth as narrow as 2 Hz.