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 or He) at specific pressures are introduced to quench fluorescence and mitigate wall relaxation. In the high-pressure limit (e.g., the N2 pressure pN2>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.
For precision atomic magnetometry, inert buffer gas is included in alkali-metal vapor cells to significantly broaden hyperfine transitions, which facilitates optical pumping and reduces diffusive relaxation, while also providing non-radiative excited state quenching. We show low-buffer gas pressure (below 50 Torr) alkali vapor cells with resolved hyperfine manifolds can also yield high-performance magnetometers. For high polarization in 87Rb, we optically pump F=2 states with narrow linewidth σ+ light, while tuning a probe beam to depopulate F=1 states (Δν=6.8 GHz from F=2). The probe tuning then also provides F=2 detection with high optical rotation and low probe broadening; we demonstrate top-bottom gradiometry, within a single 25 Torr, 0.5 cc cell, that yields an Earth's field free-precession magnetometer sensitivity of 18 fT/Hz with a 1 kHz bandwidth, as well as RF magnetometer sensitivity of 12 fT/Hz in a small band about 110 kHz.