An effect is demonstrated where off-resonant optical pumping is enhanced by spin-exchange collisions, which enables a high degree of spin orientation to be obtained in alkali-metal atoms. The experiment with room-temperature cesium vapor employs radio-frequency spectroscopy under conditions of the nonlinear Zeeman effect that allow the populations of the individual Zeeman sublevels to be determined. The improved efficiency of atomic orientation leads to a significant reduction of population relaxation out of the state with maximum magnetic quantum number
m (stretched state), which is observed as a narrowing of radio-frequency resonances. Spin-exchange collisions play a crucial role in this effect although the applied atomic density $\ensuremath{\sim}
10{}^{11}$ cm${}^{\ensuremath{-}3}$ corresponds to collision rates not greater than several tens of Hz. A simplified theoretical model has been developed to reproduce the measurement results numerically.
We present a comprehensive theory of nuclear spin polarization of
3He and
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 or
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 or
129Xe gas are assumed, namely, atmospheres of gas pressure and nearly complete quenching of the optically excited alkali-metal atoms by collisions with
N2 or
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 magnetic-resonance lines of alkali atoms are broadened considerably by the spin-exchange collisions for a radio-frequency magnetometer operating at high temperature. The resonance linewidths of cesium atoms are derived by solving the relaxation equations. When spin-exchange relaxation dominates, a light narrowing effect is predicted. For the cesium atomic radio-frequency magnetometer operates at high temperature, a remarkable narrowing of the cesium magnetic-resonance lines are observed by increasing the pump power. The Cs-Cs spin-exchange relaxation is partially suppressed by light narrowing. This study helps to expand the applications of radio-frequency magnetometers in the high-sensitivity radio-frequency magnetic-field detection.