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Physical Review A

Temperature effects in the collisional redistribution of resonance radiation in the Ba-Ar and Ba-Xe systems

Michael Scott Belsley, J. Coutts, J. Cooper

Published Oct 1, 1988• 4 citations
Publisher

Abstract

We present data on the temperature dependence of the polarization ratios of redistributed fluorescence in the Ba-Ar and Ba-Xe systems. The temperature dependence is observed to be less than 1% per 100 K, which is significantly below predicted levels.
DOI
10.1103/physreva.38.3781

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We have measured the far-wing collisional redistribution line shape, the redistributed fluorescence polarization, and the collisional alignment decay rates for barium perturbed by argon and xenon. The experiment was performed with a heated gas cell ($T\ensuremath{\sim}900$ K) with perturber-gas densities in the 1---30-Torr range and laser light detuned \ifmmode\pm\else\textpm\fi{} 3--- 1000 ${\mathrm{cm}}^{\ensuremath{-}1}$ from the 5535-\AA{} Ba I $6^{1}S\ensuremath{-}6^{1}P$ resonance line. Metal-vapor densities were determined by a Rayleigh scattering technique, which is outlined in detail. By correlating structure in the line shape with that of the polarization, we are able to make definitive statements about the interatomic potentials. The Ba data show strong similarities with previous experimental results for similar two-electron atoms, namely Ca, Sr, and Hg, and so our conclusions are of relevance to these systems as well.
The effects due to the presence of a (possibly intense) probe laser, which is used to interrogate the asymptotic excited-mj{m}_{j}mj​-state distribution resulting from the evolution through a half-collision, are systematically studied. Experimental results are obtained which are in good qualitative agreement with predictions based on a recent theoretical treatment. Finally, a simple interpretation of the relevant physical processes involved is suggested by considering the problem within a dressed-state representation.
We have made systematic measurements of the polarization of fluorescence from Sr-rare-gas systems excited off resonance by linearly polarized light. Measurements of this type give information about the evolution during a collision after the absorption of a photon. This information is important in obtaining and verifying aspects of the interaction potential that cannot be studied using conventional line-broadening experiments. We have also measured the collisional-alignment decay rates for Sr-rare-gas systems by observing the perturber-pressure dependence of the polarization of the fluorescence. To the best of our knowledge this is a new technique for measuring these decay rates.
Semiclassical formulations of collisional redistribution of polarized radiation are presented at several levels of approximation, from full classical path coupled equations to the locking/decoupling model. These are numerically tested against the results of a quantum mechanical coupled-channels formalism, by the comparison of polarization curves in both spectral wings of the Sr( 1 S 0 - 1 P 1 ) transition, with Ar and He as collisional perturbers. It is found that the locking/decoupling model can often produce good agreement with exact results if the effects due to trajectories and multiple Condon points are treated properly. Significant discrepancies due to the Condon approximation used by the model are seen in the near blue wing of the spectra and attributed to antistatic effects.