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Physical Review A

Quantum-Mechanical Transport Equation for Atomic Systems. II. Inelastic Collisions and General Line-Shape Considerations

P. R. Berman

Published Dec 1, 1972• 37 citations
Publisher

Abstract

Inelastic-collisional effects are incorporated into a quantum-mechanical transport equation (QMTE) that was developed in an earlier paper. The QMTE enables one to follow the quantum-state evolution of moving atoms which are interacting with some external fields while undergoing collisions with perturber atoms. The collisional processes are treated quantum mechanically and then reinterpreted in terms of classical variables so that the QMTE becomes an integrodifferential equation for atomic density-matrix elements containing both well-defined quantum-mechanical collision parameters (i.e., scattering amplitudes) and densitymatrix elements which are functions of classical position and velocity variables. Solutions of the QMTE enable one to derive line-shape formulas, and a discussion will be given of the general features to be expected for spectral profiles, Hanle-effect line shapes, and laser output curves, as well as the manner in which these features differ from those predicted by theories that neglect some quantum-mechanical aspects of the collision events. The inclusion of inelastic-collisional effects does not cover cases in which the frequency spacing of the atomic levels under consideration is comparable to the inverse duration time of a collision; nevertheless, the QMTE to be derived will be applicable to the analysis of a large number of atomic systems.

DOI
10.1103/physreva.6.2157

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Inelastic-collisional effects are incorporated into a quantum-mechanical transport equation (QMTE) that was developed in an earlier paper. The QMTE enables one to follow the quantum-state evolution of moving atoms which are interacting with some external fields while undergoing collisions with perturber atoms. The collisional processes are treated quantum mechanically and then reinterpreted in terms of classical variables so that the QMTE becomes an integrodifferential equation for atomic density-matrix elements containing both well-defined quantum-mechanical collision parameters (i.e., scattering amplitudes) and densitymatrix elements which are functions of classical position and velocity variables. Solutions of the QMTE enable one to derive line-shape formulas, and a discussion will be given of the general features to be expected for spectral profiles, Hanle-effect line shapes, and laser output curves, as well as the manner in which these features differ from those predicted by theories that neglect some quantum-mechanical aspects of the collision events. The inclusion of inelastic-collisional effects does not cover cases in which the frequency spacing of the atomic levels under consideration is comparable to the inverse duration time of a collision; nevertheless, the QMTE to be derived will be applicable to the analysis of a large number of atomic systems.
A quantum-mechanical transport equation (QMTE) is derived which should be applicable to a wide range of problems involving the interaction of radiation with atoms or molecules which are also subject to collisions with perturber atoms. The equation follows the time evolution of the macroscopic atomic density matrix elements of atoms located at classical position $\stackrel{\ensuremath{\rightarrow}}{\mathrm{R}}$ and moving with classical velocity $\stackrel{\ensuremath{\rightarrow}}{\mathrm{v}}$ It is quantum mechanical in the sense that all collision kernels or rates which appear have been obtained from a quantum-mechanical theory and, as such, properly take into account the energy-level variations and velocity changes of the active (emitting or absorbing) atom produced in collisions with perturber atoms. The QMTE represents a somewhat different formulation of the problem than that considered in earlier works. The present formulation is better suited to problems involving high-intensity external fields, such as those encountered in laser physics.
We present a theory of pressure effects in which the atomic center-of-mass motion is treated quantum mechanically. The quantum-mechanical calculation treats the perturber-induced energy-level variations and the velocity changes of the emitter caused by collisions on an equal basis. Specifically, we shall treat the problem of a laser to first order in the laser field, allowing for the fact that the laser atoms are undergoing collisions, but our results will also be applicable to the cases of stimulated emission or absorption. It will be sufficient to carry out a perturbation solution of the problem assuming that the laser atoms undergo at most one collision in their lifetime, since such a restricted calculation reveals the salient features of the theory. We shall find that, in general, there is no classical limit for our results. Thus, previous treatments employing a classical Boltzmann-equation approach for the atomic center-of-mass motion are invalid, and a quantum-mechanical description is necessary to correctly treat cases where both the modified Doppler effect (modified by collisions) and perturber-induced energy-level variations are present.
The work of two previous papers is extended and a theory of pressure broadening is developed which treats the perturbers quantum mechanically and allows for inelastic collisions, degeneracy, and overlapping lines. The impact approximation is used. It consists in assuming that it takes, on the average, many collisions to produce an appreciable disturbance in the wave function of the atom, and it results in an isolated line having a Lorentz shape. Validity criteria are given. When the approximation is valid, it is allowable to replace the exact, fluctuating interaction of the perturbers with the atom by a constant effective interaction. The effective interaction is expressed in terms of the one-perturber quantum mechanical transition amplitudes on and near the energy shell and its close relationship to the scattering matrix is stressed. The calculation of the line shape in terms of the effective interaction is the same as when the perturbers move on classical paths. Results are written explicitly for isolated lines. If the interaction of the perturbers with the final state can be neglected, the shift and width are proportional to the real and imaginary part of the forward elastic scattering amplitude, respectively. By the optical theorem, the width can also be written in terms of the total cross section. When the interaction in the final state cannot be neglected, the shift and width are still given in terms of the elastic scattering amplitudes, in a slightly more complicated fashion. Finally, rules are given for taking into account rotational degeneracy of the radiating states.
The effect of correlations between an absorber atom and perturbers in the binary-collision approximation are applied to degenerate atomic systems. A generalized absorption profile which specifies the final state of the atom after an absorption event is related to the total intensities of Rayleigh scattering and fluorescence from the atom. It is suggested that additional dynamical information to that obtainable from ordinary absorption experiments is required in order to describe redistributed atomic radiation. The scattering of monochromatic radiation by a degenerate atom is computed in a binary-collision approximation; an equation of motion is derived for the correlation function which is valid outside the quantum-regression regime. Solutions are given for the weak-field conditions in terms of generalized absorption and emission profiles that depend on the indices of the atomic multipoles.
In this paper, we present a formalism for the exact calculation of spectral profile of an isolated line undergoing speed-dependent collisional broadening and shifting and Dicke narrowing. It is couched in the language of the density matrix as in the closely related fields of transport phenomena, laser physics, and nonlinear optics. The formalism is ab intio in spirit, permitting the calculation of the line shape starting only from a given interaction potential. The line shape is obtained by solving a transport/relaxation equation for the off-diagonal element of the density matrix, a macroscopic quantity. The collision operator in the transport/relaxation equation, which is determined from the (microscopic) interaction between the active molecule and the perturber, is presumed known.
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.