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Physical Review A

Boltzmann-Lorentz model of collisional broadening of spectra

Sushanta Dattagupta, Łukasz A. Turski

Published Sep 1, 1985• 12 citations
Publisher

Abstract

This paper contains an analysis of a new model of collisional broadening of spectral lines in which the effect of the velocity-changing collisions is treated within the Boltzmann-Lorentz model, borrowed from the kinetic theory of gases. The simultaneous occurrence of the velocity modulations and the effects of interaction during the collisions is investigated in detail.

DOI
10.1103/physreva.32.1439

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This paper contains an analysis of a new model of collisional broadening of spectral lines in which the effect of the velocity-changing collisions is treated within the Boltzmann-Lorentz model, borrowed from the kinetic theory of gases. The simultaneous occurrence of the velocity modulations and the effects of interaction during the collisions is investigated in detail.
The shape of an isolated spectral transition is analyzed in terms of an approximation to the Waldmann–Snider kinetic equation. This equation is written in the form of a drift and collision operator acting on a density matrix. With the use of the spherical approximation, the collision operator is subdivided into an elastic Boltzmann-like collision term, an inelastic loss term, and a dephasing term. The Boltzmann-like term is responsible for Dicke narrowing of spectral lines, the inelastic loss term leads to line broadening and the dephasing term may contribute both to line broadening and shifting. Simple approximations to these terms are powerful enough to account for some of the details of experimental line shapes such as asymmetrical deviations from a Lorentzian line shape. Model numerical calculations are carried out assuming classical scattering potentials of the form 1/rn in the Boltzmann-like term and single complex frequencies for the other two. It was found that as long as the density was scaled to give the same diffusion constant, the exact form of the scattering cross section had little effect on the final line shape.
A theory of the influence of binary collisions on the line shapes associated with Doppler-free spectroscopy is presented. The specific calculation is for two-photon absorption through a real or virtual intermediate state, but the extension of the results to alternative level schemes is included. Collisions are treated quite generally at first, but, ultimately, a simple but reasonable collision model is adopted to properly account for both the "phase-interrupting" and "velocity-changing" aspects of collisions. It is shown that collisional processes can be used to distinguish between the "two-quantum" and "stepwise" contributions to the two-photon excitation rate. Moreover, it is demonstrated that systematic experimental line-shape investigations, in addition to providing tests of current collision theories, can lead to values for collision broadening and shift parameters, excitation transfer rates, magnetic substate relaxation rates, velocity-changing collision rates, and collision kernels. Consequently, Doppler-free spectroscopy can provide a new and important probe of collision effects in atomic and molecular systems.
The authors present an approach that allows the study of the influence of velocity-changing collisions (VCC) on the spectrum of resonance fluorescence. They give a theoretical framework yielding general, though quite complicated results. Working in the dressed-atom basis and describing the VCC by a strong-collision model, they focus their attention on the particular case of well separated spectral lines, which leads to relatively simple expressions. The results allow the authors to compare the effects of Doppler shifts and VCC on the profiles of the central line and on the spectra sidebands. They predict that VCC cause a narrowing of the spectral lines, which they attribute to Dicke narrowing. This prediction is also confirmed by numerical results. The adopted method of dealing with VCC in terms of collision operators can be applied to a larger class of collision models than just the strong-collision model used here.
A new approach is suggested for dealing with the many-body aspects of resonance broadening of spectral lines in gases. A Liouville-space formalism is used in which the absorption by NNN identical molecules undergoing resonance-exchange collisions is described by an NNN-dimensional projection operator in Liouville space. In the impact approximation, under conditions in which the Doppler shift of resonance frequencies can be neglected, it is shown that the effect of resonance collisions is to modify the linewidth expression obtained by ordinary foreign-gas-type theories. The shape of isolated lines remains, however, Lorentzian. Only a combined effect of Doppler and collision broadening causes appreciable deviations from the Lorentzian shape near the line center, but these deviations are not peculiar to resonance broadening.