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Journal of Physics B Atomic and Molecular Physics

Depolarisation spectra for optical collisions in the alkali-helium series

Frank Rebentrost, R. Best, Wolfgang Behmenburg

Published Jun 28, 1987• 9 citations
Publisher

Abstract

The spectra of fluorescence depolarisation (orientation, alignment) applying to single collision conditions are analysed for the alkali-helium series. These are derived from a quantum calculation of the optical collision cross sections for non-resonant collision pair excitation and include non-adiabatic couplings and thermal averaging over the collision energy. The authors find strong spectral variations of the polarisation which reflect the potential characteristics of these systems. A numerical test is performed for the classical Lewis model using realistic trajectories and a reasonable choice of the decoupling radius and fair quantitative agreement with the quantum calculation is shown. Large residual alignments in the far wings demonstrate a lack of complete reorientation of the transition dipole in a strong collision.

DOI
10.1088/0022-3700/20/12/011

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The spectra of fluorescence depolarisation (orientation, alignment) applying to single collision conditions are analysed for the alkali-helium series. These are derived from a quantum calculation of the optical collision cross sections for non-resonant collision pair excitation and include non-adiabatic couplings and thermal averaging over the collision energy. The authors find strong spectral variations of the polarisation which reflect the potential characteristics of these systems. A numerical test is performed for the classical Lewis model using realistic trajectories and a reasonable choice of the decoupling radius and fair quantitative agreement with the quantum calculation is shown. Large residual alignments in the far wings demonstrate a lack of complete reorientation of the transition dipole in a strong collision.
The fluorescence intensities for the D lines in non-resonant excitation of the alkali-helium pairs under single-collision conditions were obtained from calculations of the optical collision spectra by the quantum coupled-channels method. The close relation of the non-adiabatic transition probability from a molecular level to an atomic state during the final stage of an optical collision and the spectral dependence of the relative fluorescence intensities is investigated. An analysis of the impact region in terms of line-broadening and fine-structure cross sections calculated separately for all systems confirms the factorisation approximation.
The fluorescence intensities for the D lines in non-resonant excitation of the alkali-helium pairs under single-collision conditions were obtained from calculations of the optical collision spectra by the quantum coupled-channels method. The close relation of the non-adiabatic transition probability from a molecular level to an atomic state during the final stage of an optical collision and the spectral dependence of the relative fluorescence intensities is investigated. An analysis of the impact region in terms of line-broadening and fine-structure cross sections calculated separately for all systems confirms the factorisation approximation.
The depolarisation of the redistributed Na D1and D2line fluorescence caused by Na-Ar collisions after far-wing excitation was investigated. In the limit of zero Ar density the J=1/2orientation and J=3/2alignment reflect the distribution among Zeeman sublevels of Na 32PJproduced after absorption of a photon into one or several excited Na-Ar molecular states at small internuclear separation, followed by a mixing between these states during dissociation. Measurements of these quantities as functions of the detuning up to Delta omegaJ=50 cm-1in the red wings are compared with quantum-mechanical coupled-channel (CC) calculations using realistic molecular potentials and thermal averaging, and with predictions from the factorisation approximation (FA) of the theory of redistribution. Fair agreement with CC calculations and FA predictions was obtained within the impact region, proving the validity of the factorisation assumption there. Outside this region the overall depolarisation is primarily due to reorientation of the Na 3P electronic angular momentum and is reproduced qualitatively by the CC calculations but not by the FA theory. Additional depolarisation connected with the fine-structure coupling was observed.
Redistribution and depolarisation of light scattered by atoms undergoing collisions outside the impact region of the line profile has been studied experimentally and theoretically. In a cell experiment intensity and linear degree of polarisation of the fluorescence components 32S1/2 to or from 32P1/2,3/2 of Na atoms induced by collisions with Ar buffer gas atoms were measured as functions of the laser frequency omega L. The decrease of polarisation of the D2 component observed when omega L is shifted away from the D2 toward D1 resonance disagrees with calculations on the basis of the factorisation approximation of the theory of redistribution. Using Baylis (1975) potentials for the Na/Ar system, the effect is interpreted in terms of adiabatic coupling of the 32P3/2 electronic angular momentum to the collision axis during 'strong' collisions, giving rise to a greater than average depolarisation.
The author derives an expression for the spectrum of the radiation scattered by an atom that suffers binary collisions in the weak-field limit. The frequency of the incident radiation is in near-resonance with a multiplet transition. The authors accounts for strong atom-perturber correlations that are induced when the incident or the detected frequency is in the far wing of an absorption line. For an isolated transition between two degenerate atomic levels the model picture of quasistatic absorption followed by adiabatic reorientation of the excited state predicts a redistributed fluorescence line with a polarisation that is determined by geometrical factors.