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Physical Review

Measured Absolute Cross Sections for K* + Rb Collisional Excitation Transfer

Michael H. Ornstein, Richard N. Zare

Published May 5, 1969• 17 citations
Publisher

Abstract

The electronic excitation transfer processes, $\mathrm{K}(^{2}P_{\frac{1}{2}})\ensuremath{\rightarrow}\mathrm{Rb}(^{2}S_{\frac{1}{2}})\ensuremath{\rightarrow}\mathrm{K}(^{2}S_{\frac{1}{2}})+\mathrm{Rb}(^{2}P_{\frac{1}{2}})+\ensuremath{\Delta}E$ and $\mathrm{K}(^{2}P_{\frac{3}{2}})+\mathrm{Rb}(^{2}S_{\frac{1}{2}})\ensuremath{\rightarrow}\mathrm{K}(^{2}S_{\frac{1}{2}})+\mathrm{Rb}(^{2}P_{\frac{1}{2}})+\ensuremath{\Delta}E$ have been studied by irradiating a cell containing a nonequilibrium mixture of potassium and rubidium vapors with either the 7665 \AA{} D2 line or the 7699 \AA{} D1 line of the potassium resonance doublet. The resulting collisionally induced rubidium 7948 \AA{} fluorescence signal, isolated by interference filters used in tandem, is detected with a liquid-nitrogen-cooled $S\ensuremath{-}1$ photo-multiplier placed at right angles to the direction of excitation. Measurements of the intensity ratio of the potassium and rubidium fluoresence combined with an optical absorption determination of the rubidium atom density yields the following excitation transfer cross sections: $Q[\mathrm{K}(^{2}P_{\frac{1}{2}})\ensuremath{\rightarrow}\mathrm{Rb}(^{2}P_{\frac{1}{2}})]=2.2 {\AA{}}^{2}\ifmmode\pm\else\textpm\fi{}25%$ and $Q[\mathrm{K}(^{2}P_{\frac{3}{2}})\ensuremath{\rightarrow}\mathrm{Rb}(^{2}P_{\frac{1}{2}})]=2.6 {\AA{}}^{2}\ifmmode\pm\else\textpm\fi{}20%$ at $T=365\ifmmode^\circ\else\textdegree\fi{}\mathrm{K}\ifmmode\pm\else\textpm\fi{}2%$. Throughout an experimental run the potassium and rubidium vapor pressures are varied, but data are taken for only the lowest vapor pressures for which corrections due to resonance radiation imprisonment are unnecessary.

DOI
10.1103/physrev.181.214

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Sensitized Fluorescence in Vapors of Alkali Atoms. XIII. 62P1/2−62P3/2 Excitation Transfer in Rubidium, Induced in Collisions with Noble Gas Atoms

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The electronic excitation transfer processes, K(2P12)\ensuremath→Rb(2S12)\ensuremath→K(2S12)+Rb(2P12)+\ensuremathΔE\mathrm{K}(^{2}P_{\frac{1}{2}})\ensuremath{\rightarrow}\mathrm{Rb}(^{2}S_{\frac{1}{2}})\ensuremath{\rightarrow}\mathrm{K}(^{2}S_{\frac{1}{2}})+\mathrm{Rb}(^{2}P_{\frac{1}{2}})+\ensuremath{\Delta}EK(2P21​​)\ensuremath→Rb(2S21​​)\ensuremath→K(2S21​​)+Rb(2P21​​)+\ensuremathΔE and K(2P32)+Rb(2S12)\ensuremath→K(2S12)+Rb(2P12)+\ensuremathΔE\mathrm{K}(^{2}P_{\frac{3}{2}})+\mathrm{Rb}(^{2}S_{\frac{1}{2}})\ensuremath{\rightarrow}\mathrm{K}(^{2}S_{\frac{1}{2}})+\mathrm{Rb}(^{2}P_{\frac{1}{2}})+\ensuremath{\Delta}EK(2P23​​)+Rb(2S21​​)\ensuremath→K(2S21​​)+Rb(2P21​​)+\ensuremathΔE have been studied by irradiating a cell containing a nonequilibrium mixture of potassium and rubidium vapors with either the 7665 \AA{} D2 line or the 7699 \AA{} D1 line of the potassium resonance doublet. The resulting collisionally induced rubidium 7948 \AA{} fluorescence signal, isolated by interference filters used in tandem, is detected with a liquid-nitrogen-cooled S\ensuremath−1S\ensuremath{-}1S\ensuremath−1 photo-multiplier placed at right angles to the direction of excitation. Measurements of the intensity ratio of the potassium and rubidium fluoresence combined with an optical absorption determination of the rubidium atom density yields the following excitation transfer cross sections: Q[K(2P12)\ensuremath→Rb(2P12)]=2.2A˚2\ifmmode±\else\textpm\fi25Q[\mathrm{K}(^{2}P_{\frac{1}{2}})\ensuremath{\rightarrow}\mathrm{Rb}(^{2}P_{\frac{1}{2}})]=2.2 {\AA{}}^{2}\ifmmode\pm\else\textpm\fi{}25%Q[K(2P21​​)\ensuremath→Rb(2P21​​)]=2.2A˚2\ifmmode±\else\textpm\fi25 and Q[K(2P32)\ensuremath→Rb(2P12)]=2.6A˚2\ifmmode±\else\textpm\fi20Q[\mathrm{K}(^{2}P_{\frac{3}{2}})\ensuremath{\rightarrow}\mathrm{Rb}(^{2}P_{\frac{1}{2}})]=2.6 {\AA{}}^{2}\ifmmode\pm\else\textpm\fi{}20%Q[K(2P23​​)\ensuremath→Rb(2P21​​)]=2.6A˚2\ifmmode±\else\textpm\fi20 at T=365\ifmmode∘\else\textdegree\fiK\ifmmode±\else\textpm\fi2T=365\ifmmode^\circ\else\textdegree\fi{}\mathrm{K}\ifmmode\pm\else\textpm\fi{}2%T=365\ifmmode∘\else\textdegree\fiK\ifmmode±\else\textpm\fi2. Throughout an experimental run the potassium and rubidium vapor pressures are varied, but data are taken for only the lowest vapor pressures for which corrections due to resonance radiation imprisonment are unnecessary.
Sensitized fluorescence in rubidium vapor, induced by collisions with excited potassium atoms, was investigated to determine the total cross sections for inelastic collisions between excited potassium atoms and rubidium atoms in their ground states. The collision cross sections for the various excitation transfer processes are as follows: Q12′ (K42P1/2 → Rb52P3/2) = 40 Å2, Q22′ (K42P3/2 → Rb52P3/2) = 27 Å2, Q11′ (K42P1/2 → Rb52P1/2) = 2.7 Å2, and Q21′ (K42P3/2 → Rb52P1/2) = 1.9 Å2. The partial pressure of potassium vapor in the K–Rb mixture was kept largely below 10−5 mm Hg to eliminate effects due to the trapping of potassium resonance radiation.
Cross sections for $7^{2}D_{\frac{3}{2}}\ensuremath{\leftrightarrow}7^{2}D_{\frac{5}{2}}$ transfer in Rb, induced in collisions with He, Ne, Ar, and with ground-state Rb atoms, have been determined using methods of atomic fluorescence. Rb vapor, pure or mixed with a noble gas, was irradiated in a glass fluorescence cell with pulses of 660-nm radiation from a N2{\mathrm{N}}_{2}N2​-laser-pumped dye laser, populating one of the 2D^{2}D2D states by two-photon absorption. The resulting fluorescence included a direct component emitted in the decay of the optically excited state and a sensitized component arising from the collisionally populated state. Relative intensities of the components yielded the cross sections for 72D7^{2}D72D mixing: $Q(^{2}D_{\frac{3}{2}}\ensuremath{\rightarrow}^{2}D_{\frac{5}{2}})=8.8,6.5,10.4, \mathrm{and} 30$; $Q(^{2}D_{\frac{3}{2}}\ensuremath{\leftarrow}^{2}D_{\frac{5}{2}})=5.8,4.0,6.9, \mathrm{and} 18$, in units of ${10}^{\ensuremath{-}14}$ cm2{\mathrm{cm}}^{2}cm2 for He, Ne, Ar, and Rb, respectively. Cross sections for the effective quenching of the 2D^{2}D2D states were also determined.
Excitation transfer between the 62P126 ^{2}P_{\frac{1}{2}}62P21​​ and 62P326 ^{2}P_{\frac{3}{2}}62P23​​ resonance states in cesium, induced by Cs-N2{\mathrm{N}}_{2}N2​ and Cs-H2{\mathrm{H}}_{2}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{\mathrm{N}}_{2}N2​ collisions: ${Q}_{12}(^{2}P_{\frac{1}{2}}\ensuremath{\rightarrow}^{2}P_{\frac{3}{2}})=3.6$ A˚2{\mathrm{\AA{}}}^{2}A˚2, ${Q}_{21}(^{2}P_{\frac{1}{2}}\ensuremath{\leftarrow}^{2}P_{\frac{3}{2}})=16.2$ A˚2{\mathrm{\AA{}}}^{2}A˚2, ${Q}_{10}(^{2}S_{\frac{1}{2}}\ensuremath{\leftarrow}^{2}P_{\frac{1}{2}})=55.2$ A˚2{\mathrm{\AA{}}}^{2}A˚2, ${Q}_{20}(^{2}S_{\frac{1}{2}}\ensuremath{\leftarrow}^{2}P_{\frac{3}{2}})=63.5$ A˚2{\mathrm{\AA{}}}^{2}A˚2. For Cs-H2{\mathrm{H}}_{2}H2​ collisions: Q12=6.7{Q}_{12}=6.7Q12​=6.7 A˚2{\mathrm{\AA{}}}^{2}A˚2, Q21=29.6{Q}_{21}=29.6Q21​=29.6 A˚2{\mathrm{\AA{}}}^{2}A˚2, Q10=11.7{Q}_{10}=11.7Q10​=11.7 A˚2{\mathrm{\AA{}}}^{2}A˚2, Q20=6.7{Q}_{20}=6.7Q20​=6.7 A˚2{\mathrm{\AA{}}}^{2}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 cross sections for excitation transfer between the 62P fine structure levels of rubidium, induced in collisions with ground state rubidium atoms, have been measured using a nitrogen laser pumped dye laser as the optical excitation source in a fluorescence experiment. Rubidium vapor was irradiated with each component of the 2P rubidium doublet in turn, and measurements of the relative intensities of fluorescence yielded the following cross sections: [Formula: see text] These results are consistent with the empirical relationship between the magnitude of the cross sections and the fine structure splitting that has previously been established for the alkalis.
Cross sections for inelastic transfer between the 82D3/2 and 82D5/2 fine-structure states in rubidium, induced in resonant collisions with ground-state Rb atoms, have been determined using an experimental method involving two-photon excitation of atomic fluorescence. Rubidium vapor in a fluorescence cell was irradiated with pulses of 641 nm radiation from a N2 laser-pumped dye-laser tuned to excite one of the 82D states. The resulting fluorescence included the direct component originating from the optically excited state and a sensitized component arising from the other fine-structure state populated by collisions. Relative intensities of the fluorescent components, determined by photon-counting techniques, yielded the cross sections for excitation transfer: Q(2D3/2 → 2D5/2) = 8.1 × 10−13 cm2; Q(2D3/2 ← 2D5/2) = 5.5 × 1013 cm2; as well as [Formula: see text], the effective quenching cross section. The excitation transfer cross sections which are considered accurate to within ±20% are in the ratio predicted by the principle of detailed balancing.
The cross sections for excitation transfer between the 62P fine-structure substates in rubidium, induced in collisions with noble gas atoms, have been determined in a series of sensitized fluorescence experiments. Mixtures of rubidium vapor and noble gases at pressures varying in the range 0–5 Torr were irradiated with each component of the second 2P rubidium doublet in turn and the following cross sections for 2P mixing were obtained from measurements of sensitised-to-resonance fluorescent intensity ratios. Rb–He: Q12(2P1/2 → 2P3/2) = 29.3 Å2; Q21(2P1/2 ← 2P3/2) = 19.0 Å2. Rb–Ne: Q12 = 10.3 Å2; Q21 = 6.4 Å2. Rb–Ar: Q12 = 24.0 Å2; Q21 = 14.9 Å2. Rb–Kr: Q12 = 23.2 Å2; Q21 = 14.6 Å2. Rb–Xe: Q12 = 43.9 Å2; Q21 = 27.7 Å2 In their dependence on the magnitude of the fine-structure splitting, the values are consistent with previously determined cross sections for mixing in the first and third 2P doublets of alkali atoms.