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Physical Review A

Polarization of collisionally redistributed light from the far wings of strontium-rare-gas systems

W. J. Alford, Keith R. Burnett, J. Cooper

Published Mar 1, 1983• 51 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.27.1310

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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.
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 spectral lineshapes of the Sr (51P1–51P0) resonance transition perturbed by rare gases have been examined with a high-resolution laser-induced fluorescence method. In He and Ne, the collisional broadened spectral profiles are found to be symmetrical over the entire studied pressure range (0–600 Torr). The resulting line shapes are accurately represented by a simple Voigt profile expression. The Ar, Kr, and Xe perturbing gases, however, produce anomalous asymmetrical line broadening. To our knowledge, this represents the first measurement of asymmetrical broadening in the near wings of the emission profiles of the Sr-rare gas systems. Quantitative comparisons of the measured and theoretical line asymmetries suggest that atomic interactions in the Sr-rare gas systems are not entirely due to van der Waals (R-6)-type interactions. The line asymmetries could be caused by the correlations between thermal motions of the Sr atoms and collisional interactions.
Theory shows that to explain the polarization of light collisionally redistributed from the far line wings of an atomic transition, one must consider correlated events in which absorption during a collision, and propagation to the final Zeeman-state superposition at the end of the collision is important. Polarizations of up to about 40% have been measured in the far line wings, substantially confirming this prediction, and showing that scattering experiments cannot just be characterized by simple absorption or emission profiles.
Observations of a new dynamical process, absorption of two optical photons during a binary collision, have been made. Measurements on magnesium-rare-gas collisions display a rich phenomenology associated with the collisions, the relative linear polarization directions of the exciting light beams, and their separate detunings from atomic Mg 3s 1^{1}1S0{\mathit{S}}_{0}S0​\ensuremath{\rightarrow}3p 1^{1}1P1{\mathit{P}}_{1}P1​\ensuremath{\rightarrow}5s 1^{1}1S0{\mathit{S}}_{0}S0​ stepwise resonance. Polarization spectra for Mg-Ne and Mg-Ar fractional collisions are reported, and are seen to contain information on short-range collision dynamics and on evolution of alignment produced in the process.
The close-coupled theory of collisions in a radiation field is used to calculate the absorption profile for the Sr $^{1}\ensuremath{\leftarrow}^{1}$S resonance line broadened by collisions with Ar. The calculations predict the polarization ratios of Sr 1P^{1}\mathrm{P}1P fluorescence following line wing excitation by either linear or circular polarized light. Ab initio calculations were used to obtain the ground and excited SrAr molecular-potential curves, which were adjusted to give improved agreement with experiment. The radiative-scattering theory gives a unified description of the absorption coefficient and polarization redistribution from the small detuning impact limit region to the far spectral wings. The cross sections for elastic and inelastic depolarizing collisions of Sr 1P1^{1}\mathrm{P}_{1}1P1​+Ar were also calculated. The calculated absorption coefficient, impact-broadening rate, linear- and circular-polarization ratios, and depolarization rate coefficients are for the most part in good agreement with experiment.