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.
Theoretical and experimental presentations are given of a drastic suppression, during the interval of the excitation pulse, of forward-directed optically pumped stimulated emission from a two-photon resonantly excited state to a lower state which is also coupled to the ground state. The effect is caused by a self-induced interference from the difference-frequency mixing field that is generated during the time that the excitation fields are present. Several other implications of this effect are given and some puzzling observations in other studies are noted and clarified.
Cross sections for random collisional reorientation of J within the sublevels of the
62P23 excited state of cesium have been measured using the
D2 optical-pumping technique. The measured cross sections ${{\ensuremath{\sigma}}_{M}}^{2}$ are: Cs-He (3.2\ifmmode\pm\else\textpm\fi{}0.6)\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}15}$
cm2, Cs-Ne (2.9\ifmmode\pm\else\textpm\fi{}0.6)\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}15}$
cm2, Cs-Ar (6.0\ifmmode\pm\else\textpm\fi{}1.2)\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}15}$
cm2, Cs-Kr (9.2\ifmmode\pm\else\textpm\fi{}1.9)\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}15}$
cm2, Cs-Xe (11.3\ifmmode\pm\else\textpm\fi{}2.3)\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}15}$
cm2. Simplified equations for
D1 and
D2 pumping with zero, partial, and complete excited-state mixing are derived for a hypothetical alkali atom with zero nuclear spin. The calculations are extended to cesium atoms with nuclear spin
27 pumped by ${\ensuremath{\sigma}}^{+}$
D2 radiation. The equilibrium value
〈Sz〉0 and the time dependence
〈Sz(t)〉 of the electronic spin polarization are computed for various degrees of excited-state mixing.
〈Sz(t)〉 is found to be nearly single-exponential in the zero- and the complete-mixing cases, but shows a distinct double-exponential behavior in the intermediate region.
〈Sz〉0 is shown to be dependent on the degree of mixing, and to change sign as the degree of mixing increases. Measurements were performed with a new transmission technique by passing a separate ${\ensuremath{\sigma}}^{+}$-polarized
D2 pumping beam and an alternately ${\ensuremath{\sigma}}^{+}$- and ${\ensuremath{\sigma}}^{\ensuremath{-}}$-polarized
D1 testing beam through the cesium absorption cell. The cross sections for collisionally induced mixing were evaluated by measuring the buffer pressure at which
〈Sz〉0 passed through zero.