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Journal de physique

Light absorption by a collisional system

Henri Van Regemorter

Published Jan 1, 1987• 1 citation
Publisher

Abstract

Perturbation theory is applied to the interaction between a binary collisional system and a weak radiation field to obtain the rate of induced absorption or the line profile of an optically allowed transition at low density. The collisional system wave functions are not affected by the radiation field and appropriate different expansions of these functions must be used for the two electron-atom or atom-atom systems under study. Unified expressions of the profile are given which converges to the impact limit at small detunings. The semi-classical approach of the collisional problem is given to underline the correspondence with the usual autocorrelation formalism. Both approaches break down for large detunings where a quantum collisional theory must be used.

DOI
10.1051/jphys:019870048080129900

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Perturbation theory is applied to the interaction between a binary collisional system and a weak radiation field to obtain the rate of induced absorption or the line profile of an optically allowed transition at low density. The collisional system wave functions are not affected by the radiation field and appropriate different expansions of these functions must be used for the two electron-atom or atom-atom systems under study. Unified expressions of the profile are given which converges to the impact limit at small detunings. The semi-classical approach of the collisional problem is given to underline the correspondence with the usual autocorrelation formalism. Both approaches break down for large detunings where a quantum collisional theory must be used.
Perturbation theory for the interaction of light with a binary collisional system is applied to the calculation of line profiles, spontaneous emission rates and absorption or stimulated emission coefficients. For the usual radiation fields are perturber densities, this approximation is valid at all detunings Delta omega except the very narrow resonance region. Appropriate expansions of the total binary system wavefunctions give the emission and absorption profiles or rates, for atom-electron systems as well as for atom-atom systems, from the impact regime at small Delta omega up to the Born-Oppenheimer regime at very large Delta omega in collision-induced radiative transitions, the transitions being asymptotically allowed or forbidden. Emphasis is given to the proper averages and sums over initial and final states of the binary system which give rise to non-adiabatic effects. One shows that it is of crucial importance to include all dynamical effects during one collisional event before undertaking any calculation at small Delta omega where simultaneous collisions may occur.
Perturbation theory for the interaction of light with a binary system is applied to collisional redistribution of radiation in the weak-field limit. Within the very large domain of validity of the binary model applied to collisions between non-hydrogenic atoms and atomic perturbers at low densities, redistribution can be viewed as collisional-induced absorption followed by spontaneous decay during a second collision. The formalism can be applied from the quasimolecular domain at large detunings Delta omega 1 or Delta omega 2 up to the impact regime, but emphasis is placed here on the non-impact region, at small Delta omega 1 or Delta omega 2, where non-adiabatic effects are important in collision-induced radiative absorption or emission rates as well as in the redistribution. The impact limit of the redistribution function is easily rederived in this way.
The excitation of a two-level active atom by a radiation field in the presence of a low-density perturber bath is studied. In particular, the collisional enhancement of the absorption cross section is investigated. Features of the absorption-line profiles are predicted on physical grounds using a dressed-atom approach and verified by detailed numerical calculations for attractive, repulsive, and Lennard-Jones-type interatomic potentials. Complete spectra of the absorption cross section both as a function of detuning and as a function of field strength are given. In the weak-field limit, the results are compared with those of traditional pressure-broadening theory and to the recent experimental results of Carlsten et al. In the strong-field limit, the results display a saturation behavior consistent with the predictions of Lisitsa and Yakovlenko.
We have studied the problem of a collisionally perturbed two-level atom in an intense driving field by developing a method which allows us to calculate the field-dependent collision operator in terms of the low intensity field-independent line-broadening function arising in the usual unified theory of pressure broadening. Our relations are exact to all orders in the field in the limiting case of weak collisions, but they are exact also in the complementary case of strong collisions and weak fields. We apply our results to derive explicit expressions for the rate of optical collisions, the fluorescence spectrum in the case of well-separated components, and the absorption during an adiabatic square pulse.
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.
The formal structure of the time dependence of the state of an atom in a perturber bath in an intense classical monochromatic radiation field is studied. The authors allow the cross sections of binary collisions to be affected by the radiation field. The result is used to derive an expression for the collision-broadened saturated fluorescence excitation spectrum and absorption rate in terms of a collisional relaxation operator. This operator can be related to the rate of collisionally aided radiative excitation.