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Zeitschrift für Naturforschung A

Collisional Depolarization of Fluorescence in the Impact and Quasistatic Limit

Wolfgang Behmenburg, F. Schüller

Published Jun 1, 1977• 7 citations
Publisher

Abstract

Abstract Collisional Depolarization of fluorescence radiation has been treated by considering the impact and the quasistatic limit of the general theory of redistribution. The result shows that a variation of the degree of polarization within the fluorescence spectrum is to be expected.
DOI
10.1515/zna-1977-0606

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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.
We apply the analysis of paper I to degenerate atomic systems and calculate the effect of correlations between an atom (the absorber) and perturbers in the binary-collision approximation. The result of our calculation is a generalized absorption profile that specifies the final state of the atom an absorption event. This profile is then related to the total intensities of Rayleigh scattering and fluorescence (redistributed radiation) from the atom. The profile is expressed in terms of collision operators that depend on the index of the multipole of the atom that is created. Some of the operators represent correlations between radiative and collisional events and cannot, except in certain limits, be expressed in terms of the usual line-broadening operators. This, of course, implies that one needs extra dynamical information, on top of that obtainable from ordinary absorption experiments, to be able to describe redistribution. Conversely, redistribution offers a probe of collisional dynamics, not given by absorption experiments, via the polarization of fluorescent light. We give practical expressions for the calculation of these operators and discuss their implications.
Energy transfer and coherence transfer between two atoms of different species are studied theoretically. The electric dipole-dipole interaction is the mechanism considered for the excitation transfer. A generalized perturbation method for a damping system is used. A general formula is derived for the polarization of the sensitized fluorescence resulting from the excitation transfer. This polarization is shown to be dependent on the angular momenta of the two atoms, and to be independent of their relative velocity as well as of their difference in the energy of excitation. The polarizations are found to be nonzero in many cases which demonstrate the transfer of coherence through collision processes. A general and compact formula is also derived for the polarization of pure fluorescence where excitation exchange has not taken place. The polarization of the sensitized fluorescence is in general smaller than that of the pure fluorescence. This means that the coherence is transferred only partially. Finally, the magnetic field effect has been included. This field depolarization depends on the gj{g}_{j}gj​ values and the lifetimes of the excited states of both atoms. The general feature of the field dependence also differs considerably from that of the Hanle effect for resonance fluorescence.
By means of the selection rule Σ m J = constant along the axis of a collision between two atoms, it is shown that sensitized fluorescence should in some cases be partially polarized. The degree of polarization of the fluorescence of cadmium vapour sensitized by the presence of mercury vapour is calculated for certain states of polarization of the incident radiation. In the case studied experimentally the degree of polarization varies over a range of 2-5%. The theoretical value is 3/11, which is reduced in practice by various depolarizing effects. The possibility of transfer coherence between eigenstates from mercury to cadmium during a collision is considered.
The polarization properties of excited alkali atoms having suffered half collisions with noble gas atoms following excitation by nonresonant photon absorption during a strong collision, are investigated. On the basis of a semiclassical perturbation treatment of the density matrix up to second order in the driving field a general expression for the polarization dependent intensity of the emitted alkali fluorescence is derived. Assuming quasistatic excitation of the collision complex and considering reorientation of the orbital and spin electronic angular momenta within a cut off radius, explicit results for the polarization degrees are presented and discussed, depending on the initial molecular excited state and coupling case.