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.
6 2P1/2 ↔ 6 2P3/2 mixing and 6 2S1/2 ← 6 2P1/2,3/2 quenching in cesium, induced in collisions with ground state N2, H2, HD, and D2 molecules, have been investigated using techniques of sensitized fluorescence. Mixtures of cesium vapor and the gases, in which the cesium vapor pressure was kept very low to avoid multiple scattering, were irradiated with each component of the cesium resonance doublet in turn. The fluorescence which contained both components of the doublet was observed in a direction perpendicular to that of the exciting beam. Measurements of the relative intensities of the fluorescent components yielded the following cross sections for mixing and quenching. For Cs–N2 collisions: Q12(2P1/2 → 2P3/2) = 4.7 Å2, Q21(2P1/2 ← 2P3/2) = 25 Å2, Q10(2S1/2 ← 2P1/2) = 77 Å2, Q20(2S1/2 ← 2P3/2) = 69 Å2. For Cs–H2 collisions: Q12 = 6.7 Å2, Q21 = 44 Å2, Q10 = 7 Å2, Q20 = 5 Å2. For Cs–HD collisions: Q12 = 4.8 Å2, Q21 = 32 Å2, Q10 = 4 Å2, Q20 = 3 Å2. For Cs–D2 collisions: Q12 = 4.2 Å2, Q21 = 28 Å2, Q10 = 8 Å2, Q20 = 7 Å2. The Cs–N2 and Cs–H2 cross sections supersede the values published previously (McGillis and Krause 1967). The cross sections Q21 appear to exhibit resonances with molecular rotational transitions.
Excitation transfer between the
62P21 and
62P23 resonance states in cesium, induced by Cs-
N2 and Cs-
H2 collisions, was observed in the first experiment of its kind, in which techniques of sensitized fluorescence are used to investigate collisional mixing between resonance states of alkali atoms in mixtures with molecular gases. The cesium-vapor-gas system, in which the cesium vapor pressure was low enough to avoid radiation trapping, was irradiated with a single component of the resonance doublet. The fluorescent light, which contained both components of the doublet, was monitored at right angles to the direction of excitation. Measurements of relative intensities of the fluorescent components yielded the following cross sections for excitation transfer and for quenching of resonance radiation. For Cs-
N2 collisions: ${Q}_{12}(^{2}P_{\frac{1}{2}}\ensuremath{\rightarrow}^{2}P_{\frac{3}{2}})=3.6$
A˚2, ${Q}_{21}(^{2}P_{\frac{1}{2}}\ensuremath{\leftarrow}^{2}P_{\frac{3}{2}})=16.2$
A˚2, ${Q}_{10}(^{2}S_{\frac{1}{2}}\ensuremath{\leftarrow}^{2}P_{\frac{1}{2}})=55.2$
A˚2, ${Q}_{20}(^{2}S_{\frac{1}{2}}\ensuremath{\leftarrow}^{2}P_{\frac{3}{2}})=63.5$
A˚2. For Cs-
H2 collisions:
Q12=6.7 A˚2,
Q21=29.6 A˚2,
Q10=11.7 A˚2,
Q20=6.7 A˚2. The large sizes of the excitation-transfer cross sections, which are comparable to the corresponding Cs-Cs cross sections, are attributed to resonances with transitions in the molecules.
The impact broadening of Na(nP1/2) (n=6-24), K(nP1/2) (n=8-24) and Rb(nP12/) (n=10-24) levels by noble-gas atoms, N2 molecules and alkali atoms in the ground state has been investigated. Broadening cross sections have been evaluated on the grounds of contributions coming from Rydberg-electron-perturber and ionic core-perturber scattering. Broadening cross sections for Cs(nD3/2)+Cs(6S) collisions for n=11-23 have also been calculated to compare with the experimental ones. Theoretically evaluated broadening cross sections for K(nP12/)+K(4S) and Cs(nD3/2)+Cs(6S) collisions appeared to be in good agreement with existing experimental data.