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The Journal of Chemical Physics

Quenching of electronically excited barium atoms, Ba(5d 3D J)

Peter G. Whitkop, J. R. Wiesenfeld

Published Jan 15, 1980• 22 citations
Publisher

Abstract

The lowest optically metastable excited state of barium, Ba(5d 3DJ), was populated by laser excitation of the 6p 1P01←6s 1S0 (λ=553.5 nm) transition followed by the spontaneous emission 6p 1P01→5d 3DJ (λ∼1130 nm). No evidence for the normally spin allowed transition 6p 1P01 →5d 1D2 (λ=1500 nm) was obtained. The deactivation of Ba (5d3DJ) by Ba (6s 1S0) is extremely efficient proceeding with a thermal cross section of 1.3±0.1 nm2 at ?730 K. This is in sensible accord with recent calculations of Ba2 potential curves.

DOI
10.1063/1.439192

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The lowest optically metastable excited state of barium, Ba(5d 3DJ), was populated by laser excitation of the 6p 1P01←6s 1S0 (λ=553.5 nm) transition followed by the spontaneous emission 6p 1P01→5d 3DJ (λ∼1130 nm). No evidence for the normally spin allowed transition 6p 1P01 →5d 1D2 (λ=1500 nm) was obtained. The deactivation of Ba (5d3DJ) by Ba (6s 1S0) is extremely efficient proceeding with a thermal cross section of 1.3±0.1 nm2 at ?730 K. This is in sensible accord with recent calculations of Ba2 potential curves.
An observation of light-induced drift (LID) of atoms with an intermediate metastable level between the ground and excited resonance levels is reported. The drift of atoms of barium was investigated. Molecular nitrogen was used as a buffer gas. The 5d 1^{1}1D metastable state of Ba atoms was quenched in collisions with N2{\mathrm{N}}_{2}N2​ molecules. It has been deduced from the experimental results that the collision cross section of Ba atoms with N2{\mathrm{N}}_{2}N2​ molecules is larger for Ba atoms in the ground state than in the 6p 1^{1}1P excited state. The maximal LID velocity was about 250 cm/s.
This is the first reported demonstration of the use of pair-absorption transitions for optically pumping lasers. In a mixture of barium and thallium metal vapors, single-photon absorption of 3867-A laser light caused simultaneous excitation of colliding ground-state atoms to the Ba(6s6p 1P1(o)) and Tl(6p 2P(3/2)(o)) excited states. Excited-state densities of about 10(14) cm(-3) were created, and subsequent laser emission on the Ba(6s6p 1PI(o)) - Ba(6s5d 1D2) atomic transition at 1.5 microm was observed.
Abstract The kinetics of two-step photoionization of barium atoms through excited P 1 1 , 3 levels was studied by numerical simulation method in the optically dense approximation. The first laser at wavelength λ 1 = 553.5 nm ( λ 1 = 791 nm) pumps transition S 0 1 ↔ P 1 1 ( S 0 1 ↔ P 1 3 ). The second laser with λ 2 = 266 nm ( λ 2 = 310 nm) ionizes atoms from the level P 1 1 ( P 1 3 ). The third probe laser with wavelength λ i = 493.41 nm causes resonant fluorescence of barium ions. It is shown that the metastable D 2 3 from the D 1 , 2 , 3 3 triplet in barium is strongly populated through P 1 <
Time-resolved measurements of fluorescence and level populations have been made on barium vapour illuminated by an intense pulse of laser radiation (1 MW cm -2 , 50 ns FWHM) tuned to the resonance transition of Ba I, 6s 2 1 S 0 -6s6p 1 P 1 , at 5535 AA. Barium number densities between 10 13 -10 15 cm -3 were investigated, using a buffer gas of helium at 100 Torr. Fluorescence was measured with two different geometrical arrangements, one allowing partial spatial resolution. In neither case did the observed fluorescence saturate with increasing laser power, although the maximum flux was more than sufficient to burn through the vapour column, as confirmed by transmission measurements. The power loss from the laser beam was found to be compatible with the scattered radiation from the pumped column in the absence of radiation trapping. In contrast to other similar experiments, no significant ionisation was detected (<5%). Time-resolved population measurements by anomalous dispersion on the 6s6p 3 P 2 and 6s5d 1 D 2 metastable levels yielded quenching cross sections for both Ba-Ba and Ba-He collisions, but gave anomalous result for the peak populations. A qualitative explanation of the fluorescence anomaly is proposed on the basis of the AC Stark effect, and it is shown that the same effect can inhibit the onset of stimulated emission to the metastable D levels.