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Canadian Journal of Physics

Theory of excitation transfer in collisions between alkali atoms. I. Identical partners

E. I. Dashevskaya, A. Voronin, E. E. Nikitin

Published Jun 15, 1969• 78 citations
Publisher

Abstract

A mechanism is derived for nonresonant transfer of electronic excitation energy, induced in the process M*(2P3/2) + M(2S1/2) → M*(2P1/2) + M(2S1/2), where M and M* are identical alkali atoms in the ground and first excited states, respectively. Various types of interactions, responsible for the nonadiabatic combination of electronic states of the quasi molecule M2*, were considered, and their respective contributions to the cross section for excitation transfer were determined.

DOI
10.1139/p69-157

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Inelastic collisions between excited alkali atoms and molecules. V. Sensitized fluorescence in mixtures of sodium with N2, H2, HD, and D2

M. Stupavsky, L. Krause

3 2P1/2 ↔ 3 2P3/2 excitation transfer in sodium, induced in inelastic collisions with ground-state N2, H2, HD, and D2 molecules, has been investigated in a series of sensitized fluorescence experiments. Mixtures of sodium vapor at a pressure of 5 × 10−7 Torr, and the gases, were irradiated with each NaD component in turn, and the fluorescence which contained both D components was monitored at right angles to the direction of the exciting beam. Measurements of the relative intensities of the NaD fluorescent components yielded the following collision cross sections for excitation transfer. For Na–N2 collisions: Q12(2P1/2 → P3/2) = 144 Å2, Q21(2P1,2 ← 2P3/2) = 76 Å2 for Na–H2 collisions: Q12 = 80 Å2, Q21 = 42 Å2. For Na–HD collisions: Q12 = 84 Å2, Q21 = 44 Å2. For Na–D2 collisions: Q12 = 98 Å2, Q21 = 52 Å2. The cross sections Q21 exhibit a slight resonance effect between the atomic and molecular rotational transitions.

Canadian Journal of Physics•Oct 1, 1968•23 citations
A mechanism is derived for nonresonant transfer of electronic excitation energy, induced in the process M*(2P3/2) + M(2S1/2) → M*(2P1/2) + M(2S1/2), where M and M* are identical alkali atoms in the ground and first excited states, respectively. Various types of interactions, responsible for the nonadiabatic combination of electronic states of the quasi molecule M2*, were considered, and their respective contributions to the cross section for excitation transfer were determined.
The total cross sections for excitation transfer between the 6 2P1/2 and 6 2P3/2 levels in cesium, induced by collisions of the second kind between cesium and inert gas atoms, have been determined using methods of sensitized fluorescence. The experiments were carried out at a cesium vapor pressure of 1 × 10−6 mm Hg, at which there is no trapping of resonance radiation, and over a range of inert gas pressures extending from 1 to 300 mm Hg. The cross sections Q1(2P1/2 → P3/2) and Q2(2P1/2 ← 2P3/2) are as follows: Cs–He: 5.7 × 10−21 and 3.9 × 10−20 cm2; Cs–Ne: 1.9 × 10−21 and 3.1 × 10−20 cm2; Cs–A: 1.6 × 10−21 and 5.2 × 10−20 cm2; Cs–Kr: 8.3 × 10−21 and 18.4 × 10−20 cm2; Cs–Xe: 7.2 × 10−21 and 27.4 × 10−20 cm2. A mechanism for the excitation transfer is suggested, which involves an interaction between the inert gas atoms and the 6 2P electron in cesium, behaving as a free particle.
An account of recent work is given by the author and co-workers on the experimental determination of cross sections for excitation transfer between the (2)P((1/2)) and (2)P(3/2)resonance levels in potassium, rubidium and cesium, induced by inelastic collisions with alkali atoms and inert gas atoms in their ground states. Forty values of cross sections were obtained in a series of sensitized fluorescence experiments, in which alkali vapors and vapor-gas mixtures were irradiated with one component of the appropriate alkali resonance doublet, and the relative intensities of both components appearing in the fluorescent light were measured. The experiments indicate that the collisional interaction between an alkali atom in a (2)P state and a ground state inert gas atom probably occurs between the inert gas atom and the (2)P alkali valence electron which behaves like a quasi-free particle.
Sensitized fluorescence in cesium vapor induced by collisions with excited rubidium atoms was investigated in order to determine the total cross sections for inelastic collisions between excited rubidium atoms and cesium atoms in their ground states. The partial pressure of the rubidium vapor in the Rb–Cs mixture was kept below 2 × 10−5 mm Hg in order to eliminate effects due to the trapping of the Rb resonance radiation. The collision cross sections for the various excitation transfer processes are as follows: Q12′(Rb 5 2P1/2 → Cs 6 2P3/2) = 1.5 Å2; Q11′(Rb 5 2P1/2 → Cs 6 2P1/2) = 0.5 Å2; Q22′(Rb 5 2P3/2 → Cs 6 2P3/2) = 0.9 Å2; Q21′(Rb 5 2P3/2 → Cs 6 2P1/2) = 0.3 Å2. The fact that the cross sections are considerably smaller than those for collisions between similar atoms indicates that the Rb–Cs interactions probably involve van der Waals' forces with a much shorter range than exchange forces, which play a dominant role in Rb–Rb or Cs–Cs collisions.
3 2P1/2 ↔ 3 2P3/2 excitation transfer in sodium, induced in inelastic collisions with ground-state N2, H2, HD, and D2 molecules, has been investigated in a series of sensitized fluorescence experiments. Mixtures of sodium vapor at a pressure of 5 × 10−7 Torr, and the gases, were irradiated with each NaD component in turn, and the fluorescence which contained both D components was monitored at right angles to the direction of the exciting beam. Measurements of the relative intensities of the NaD fluorescent components yielded the following collision cross sections for excitation transfer. For Na–N2 collisions: Q12(2P1/2 → P3/2) = 144 Å2, Q21(2P1,2 ← 2P3/2) = 76 Å2 for Na–H2 collisions: Q12 = 80 Å2, Q21 = 42 Å2. For Na–HD collisions: Q12 = 84 Å2, Q21 = 44 Å2. For Na–D2 collisions: Q12 = 98 Å2, Q21 = 52 Å2. The cross sections Q21 exhibit a slight resonance effect between the atomic and molecular rotational transitions.