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Physical Review A

Influence of atomic coherence induced by laser-assisted near-resonant collisions on the far-wing absorption profile

Józef Szudy, W. E. Baylis

Published Apr 1, 1996• 0 citations
Publisher

Abstract

An analysis of near-resonant collisions between dissimilar atoms in the presence of a radiation field reveals their effect on the far wings of the absorption profile. Extending a model due to Cavalieri, Arimondo, and Matera, we take into account the collisional shifts of atomic levels, as well as the collisional coupling between atoms and the coupling with the radiation field. A general formula for the absorption profile is derived and expressed in terms of the universal line-shape function of the unified Franck-Condon treatment of pressure broadening. We show that in some cases collision-induced coherence can give rise to a strongly depressed red wing that exhibits transparency for some values of the laser detuning. \textcopyright{} 1996 The American Physical Society.

DOI
10.1103/physreva.53.2539

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An analysis of near-resonant collisions between dissimilar atoms in the presence of a radiation field reveals their effect on the far wings of the absorption profile. Extending a model due to Cavalieri, Arimondo, and Matera, we take into account the collisional shifts of atomic levels, as well as the collisional coupling between atoms and the coupling with the radiation field. A general formula for the absorption profile is derived and expressed in terms of the universal line-shape function of the unified Franck-Condon treatment of pressure broadening. We show that in some cases collision-induced coherence can give rise to a strongly depressed red wing that exhibits transparency for some values of the laser detuning. \textcopyright{} 1996 The American Physical Society.
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.
General expressions are derived for the spectral line shapes of resonance absorption and scattering of coherent radiation in collision-broadened gases, taking into account effects of coherent excitation of two or more atoms (or molecules), as steady-state solutions of a hierarchy of master equations described in a previous publication (paper I). Coupling between the coherent motions of the atoms, provided by a Bethe-Salpeter---type effective interaction, in the binary-collision approximation, forms the essential mechanism for introducing cooperative coherent effects into the steady-state spectra. Explicit expressions are given for the effects of two-atom coherence in the binary-collision approximation, in which the Bloch-type dressed-atom self-energy superoperator is modified by the presence of collisions in which both atoms retain memory of their coherent propagation before the collision. The self-energies include the effects of resonance exchange symmetrization in self-broadening, and are renormalized by the coincidence of radiative transitions during the collisions. The impact (near-resonance) and the quasistatic (line-wing) limits of the applied-frequency detunings are discussed. In the quasistatic limit, coherent many-atom excitations become irrelevant; however, interactions of both collision partners with the radiation during the collision accounts for such phenomena as collision-induced absorption or radiative collisions. In the impact limit, the inclusion of the Bethe-Salpeter interactions allows for the appearance of two-atom resonances. Magnitude estimates of these effects are discussed. Effects of higher-rank (many-body) coherences are formally discussed with the help of a diagrammatic method, leading into implicit bootstrap equations that can be solved by iterative or other procedures.
An absorption (and/or emission) event which takes place during a strong collision is called a 'correlated event'. It is discussed how correlated events affect the far red wing depolarization of fluorescence. Attention is given to an atomic vapor which is irradiated by linearly polarized light of a frequency on the red side of the resonance line. Two limiting cases are considered, corresponding to excitation in the impact region and in the quasi-static wing. In the quasi-static wing, absorption of a photon followed by fluorescence (rather than Rayleigh scattering), occurs mostly during a collision. Correlated events dominate the scattering process. Expressions derived for the polarization of the fluorescent light are applied to far red wing depolarization. It is found that the polarization of the fluorescent light does not go to zero in the far wing, but depends crucially on the detailed nature of the anisotropy in the long-range part of the interatomic potential.
The collisionally broadened optical absorption cross section that is constant at low intensities is predicted to decrease at high intensities. The prediction is based on a nonlinear change of the effective interaction of the atom with the strong incident electromagnetic field and a distortion of the atomic interaction potential by it. An experiment is analyzed here that observes this falloff on the “wing” of the 460.73-nm strontium resonance line, collision broadened by an argon buffer gas. Qualitative agreement is reached between theory and experiment when the degeneracy of the levels is taken into account.