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.
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
2P21 and
2P23 first excited states is relatively large, allowing the isolation of mixing effects within a particular
J 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
J-state sublevels have been calculated for an alkali atom of nuclear spin
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.
The standard model of Spin-Exchange Optical Pumping of 3 He has come under close scrutiny as researchers try to maximize the quantity and polarization of 3 He. This paper will review four important effects that have come to light: 1) pumping with frequency narrowed diode lasers significantly improves the polarization and production rate as compared to off-the-shelf broadband sources 2) Rb-K mixtures again improve the production rate due to reduced collisional loss in K-He collisions, 3) a unexplained 3 He wall relaxation mechanism that scales closely with alkali vapor pressure limits the attainable 3 He polarization to about 80%, 4) a small collisionally-induced breakdown in the selection rules for optical pumping explains why narrowband lasers are so advantageous, and may explain some observed limitations for Rb-K pumping as well.
We demonstrate spin-exchange optical pumping of
3He using a ``hybrid'' K-Rb vapor mixture. The Rb atoms absorb light from a standard laser at 795 nm, then collisionally polarize the potassium atoms. Spin-exchange collisions of K and
3He atoms then transfer the angular momentum to the
3He with much greater efficiency than $\mathrm{R}\mathrm{b}\mathrm{\text{\ensuremath{-}}}^{3}\mathrm{H}\mathrm{e}$. For a K-rich vapor, the efficiency of the hybrid spin-exchange collisions approaches
1/4, an order of magnitude greater than achieved by pure Rb pumping. We present the first measurements of actual photon efficiencies (polarized nuclei produced per absorbed photon), and show that a new parasitic absorption process limits the total efficiencies for both hybrid and pure Rb pumping.
We present measurements of the circular dichroism of optically pumped Rb vapor near the
D1 resonance line. Collisions with the buffer gases
3He and
N2 reduce the transparency of the vapor, even when fully polarized. We use two methods to measure this effect, show that the He results can be understood from RbHe potential curves, and show how this effect conspires with the spectral profile of the optical pumping light to increase the laser power demands for optical pumping of very optically thick samples.
Cross sections for
72D and
82D fine-structure mixing in Rb, induced by collisions with various ground-state atoms and
N2 molecules, have been determined using methods of atomic fluorescence. Rb vapor, pure or mixed with a buffer gas, was irradiated in a glass fluorescence cell with pulses of radiation from a
N2 laser-pumped dye laser, populating a
2D fine-structure state by two-photon absorption. The resulting fluorescence included a direct component arising from the optically excited state and a sensitized component due to the collisionally populated fine-structure state. Measurements of relative intensities of the two components in relation to buffer-gas pressure yielded the following cross sections (in units of ${10}^{\ensuremath{-}14}$
cm2): $Q({7}^{2}{D}_{\frac{3}{2}}\ensuremath{\rightarrow}{7}^{2}{D}_{\frac{5}{2}})=14.1,15.5,\mathrm{and}10.0$; $Q({7}^{2}{D}_{\frac{3}{2}}\ensuremath{\leftarrow}{7}^{2}{D}_{\frac{5}{2}})=9.0,10.5,\mathrm{and}6.9$, for Kr, Xe, and
N2, respectively; $Q({8}^{2}{D}_{\frac{3}{2}}\ensuremath{\rightarrow}{8}^{2}{D}_{\frac{5}{2}})=8.9,4.9,12.4,24.9,25.8,12.1,\mathrm{and}43.1$; $Q({8}^{2}{D}_{\frac{3}{2}}\ensuremath{\leftarrow}{8}^{2}{D}_{\frac{5}{2}})=5.8,3.2,9.4,15.1,17.6,8.3,\mathrm{and}28.5$, for He, Ne, Ar, Kr, Xe,
N2, and Rb, respectively. Cross sections for the effective depopulation of the
2D states were also determined.