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Journal of Physics B Atomic and Molecular Physics

Laser selective excitation of a three-level atom: Barium

John L. Carlsten

Published Sep 11, 1974• 23 citations
Publisher

Abstract

A simple theory describing selective excitation of a three-level atom with a tuneable laser is developed. Effects of number density, line widths and laser parameters on the final populations of the levels with laser excitation are discussed. An experiment is described in which a tuneable dye laser is used to pump large numbers of barium atoms into the 6s5d 3 D metastable term from the (bs) 2 1 S 0 ground state via the 6s6p 3 P term. The theory for the interaction of the laser with this 'three-level system' predicts that approximately 80% of the barium atoms should be excited into the 3 D term. Experimentally the largest amount of excitation to the 3 D term observed was (78+or-5)%.

DOI
10.1088/0022-3700/7/13/008

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Physica Scripta•Dec 19, 2022•0 citations
A simple theory describing selective excitation of a three-level atom with a tuneable laser is developed. Effects of number density, line widths and laser parameters on the final populations of the levels with laser excitation are discussed. An experiment is described in which a tuneable dye laser is used to pump large numbers of barium atoms into the 6s5d 3 D metastable term from the (bs) 2 1 S 0 ground state via the 6s6p 3 P term. The theory for the interaction of the laser with this 'three-level system' predicts that approximately 80% of the barium atoms should be excited into the 3 D term. Experimentally the largest amount of excitation to the 3 D term observed was (78+or-5)%.
An experiment is described in which large numbers ( approximately 10 16 ) of calcium atoms are placed in the 4s4p 3 P metastable level by optical pumping with a tunable dye laser and then studied spectroscopically. Equations governing the degree of excitation by the laser are derived. Predictions of the theory are shown to be in good agreement with experimental results. In particular, at low optical depths produced by 10 15 ground state atoms cm -2 the dye laser raises approximately 50% of the calcium atoms into the metastable state. At higher optical depths associated with 10 17 ground state atoms cm -2 the number of excited states is limited only by the laser energy and line width. For the dye laser used the largest number of metastables produced was approximately 10 16 . The absorption spectra of the 4s4p 2 P level is seen out to 4s4p 3 P to 4s22d 3 D. The relaxation rate between the excited state fine structure is studied directly with an optically delayed dye laser continuum. Other applications of this technique of producing large numbers of excited states are briefly discussed.
We demonstrate an experimental technique that selects the nuclear spin I=0 isotope 138Ba^{138}\mathrm{Ba}138Ba for spectroscopic measurements from a beam of natural barium containing seven stable isotopes. A cw dye laser is used to optically pump the I=3/2 isotopes 135Ba^{135}\mathrm{Ba}135Ba and 137Ba^{137}\mathrm{Ba}137Ba into the metastable 6s5d 1^{1}1D2{\mathit{D}}_{2}D2​ and 3^{3}3D1,2{\mathit{D}}_{1,2}D1,2​ levels via the 6s6p 1^{1}1P1{\mathit{P}}_{1}P1​ excited state, leaving nearly pure 138Ba^{138}\mathrm{Ba}138Ba in the ground state. Photoionization spectra of the excited 5d6p 3^{3}3D1{\mathit{D}}_{1}D1​ even isotope state recorded with optical pumping of 135Ba^{135}\mathrm{Ba}135Ba and 137Ba^{137}\mathrm{Ba}137Ba to the metastable levels are essentially devoid of forbidden features associated with the hyperfine interaction in the odd isotopes.
Shift and broadening parameters for doubly excited states of 5d6d, 5d7d, 5d7s, 5d8s and 6p 2 configurations in neutral barium atoms are presented. A tunable dye laser pumped by an excimer laser was used to populate the Rydberg states of Ba by two-photon absorption from the 6s 2 1 S 0 ground state. Inert gases Ar, Kr and Xe at 100 mbar pressure were used as perturbing gases. The resulting line shapes were fitted to a Voigt line shape function, from which shift and broadening parameters were inferred.
Energy-pooling collisions between low-lying excited states of Ba have been studied. We have used a CW dye laser to excite the level in Ba. Radiative decay and collisions with Ba or buffer-gas atoms (Ar, He) populate also the , and metastable levels. The spatial density distributions of these excited levels were measured by the absorption of lines from a Ba hollow-cathode lamp as a function of laser frequency. When the laser was on the exact atomic resonance we observed fluorescence from the , , , , , , and states populated by energy-pooling collisions of Ba( , ). By changing the buffer gas pressure the fluorescence intensity ratio between - and - transitions changes dramatically. This is found to be due to redistribution of population among metastable levels, both in magnitude and space. In addition, we have found that the and metastable levels are also populated when the laser is tuned to the blue from the 553.5 nm line under which conditions a pronounced red-shifted light cone (cone emission) is 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 <