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Soviet Journal of Quantum Electronics

A contribution to the theory of resonant two-photon absorption in a gas

Э. Г. Сапрыкин, Gennady I. Smirnov

Published Mar 31, 1976• 0 citations
Publisher

Abstract

A solution is obtained to the problem of the influence of level degeneracy and depolarizing collisions on the form of the spectrum of resonant two-photon absorption in gases. It is shown that such absorption may provide an effective method for the determination of the decay constants of multipole moments of electron shells. It is also demonstrated that the determination of the impact broadening parameters can be simplified by the use of an external magnetic field.

DOI
10.1070/qe1976v006n03abeh011084

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A solution is obtained to the problem of the influence of level degeneracy and depolarizing collisions on the form of the spectrum of resonant two-photon absorption in gases. It is shown that such absorption may provide an effective method for the determination of the decay constants of multipole moments of electron shells. It is also demonstrated that the determination of the impact broadening parameters can be simplified by the use of an external magnetic field.
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A detailed analysis is made of transient coherent Doppler-free spectroscopy of two-photon absorption in an atomic gas. The hyperfine structure of the levels and elastic depolarizing collisions are allowed for. The analysis is used to develop a method for the determination of the time constant of relaxation of the multipole moments of atoms when such relaxation is due to radiative decay and collisions with a buffer gas. A way of determining the separation between the hyperfine structure components is demonstrated. It is shown that under conditions of excitation of the atoms the hyperfine structure of the levels can give rise to quantum beats of the density of a conjugate wave.
Non-stationary two-photon absorption coherent spectroscopy free of Doppler broadening in an atomic gas has been considered in detail. Correct account has been taken of the level degeneracy and depolarizing collisions. This two-photon Doppler-free spectroscopy has been developed for determining the relaxation rates of the atomic multipole moments in gas. A criterion to test the adopted model of the depolarizing collisions has been developed. A possible method for the identification of the atomic transitions in the angular momentum has been formulated. A technique of precisely determining the separation between the energy levels of the two-photon transition has been proposed. The conditions under which the Stokes wave is conjugated with respect to the probe pulse in amplitude, phase and polarization have been determined for the atomic gas in the presence of depolarizing collisions.
Using the exact solution for a sine-driven two-level system we have calculated the nonlinear absorption coefficient of a gas of two-level molecules with homogeneous (hard collisions, spontaneous decay) and inhomogeneous (Doppler effect) broadening mechanisms. We have studied the dependence of the form of the absorption lines on relaxation parameters, on the strength of the electric field, and for various ratios between the homogeneous and inhomogeneous linewidths. We include considerations about saturation of the medium caused by the external field that gives rise to the so-called power broadening of the spectral lines. The dependence of the linewidth on the saturation parameters and on the relaxation parameters is determined. These parameters appear in the ratio of the purely homogeneous and purely inhomogeneous linewidths. Asymptotic behaviors of this linewidth for the homogeneous limit and for the inhomogeneous limit are also determined.
In the limit of a dipole-dipole interaction between neutral atoms and the binary-collision approximation, we present a theory of pressure broadening in which the multiplet structure of the atomic levels is considered. The appropriate Schr\"odinger equations for the collision problem are numerically integrated to obtain solutions for both resonant and foreign gas broadening. The presence of radiation fields is neglected in the first half of the paper, where the collisional time rate of change of the density matrix is found. The pertinent collisional decay parameters are extracted from these equations. The ratios of the parameters of the average magnetic dipole to electric quadrupole moment obtained were 1.21\ifmmode\pm\else\textpm\fi{}0.02 for the relaxation of the entire ensemble in resonant broadening, 0.966\ifmmode\pm\else\textpm\fi{}0.012 for the relaxation of the initially excited atoms in resonant broadening, and 1.12\ifmmode\pm\else\textpm\fi{}0.02 for the relaxation of the initially excited atoms in foreign gas broadening. In the second half of the paper, the collisional broadening results are incorporated in a systematic evaluation of (i) spectral profiels (effects arising from the velocity and recoil of the emitting atom are neglected), (ii) Hanle-effect line shapes, and (iii) laser phenomena. For the case of resonant broadening, the radiation trapping process is reviewed and its influence on line shapes discussed. Finally, a detailed comparison of the theory with experimental findings as well as with previous theoretical results is made. We conclude that the dipole-dipole interaction is sufficient to explain most cases of resonant and some cases of foreign gas broadening.
The theory of interaction of intense bichromatic field of laser radiation with multilevel atomic system in the external magnetic field is considered. The magnitudes of interaction are much larger than the width of atomic levels. The vector-potential of radiation field consisting of two monochromatic components with the frequencies resonant to adjacent transitions is taken in electric dipole approximation. The eigenvalues and eigenstates of the Hamiltonian, including spin-orbit interaction and interactions with laser radiation and external magnetic fields, are found without perturbation theory using resonant approximation. When the effects of resonantly excited radiation are considered the Hamiltonian of interaction with the weak field of scattered radiation is included also. Its eigenfunctions are found with the help of perturbation theory. We consider tow types of effects: polarization effects and effects of resonantly excited radiation. As the atomic system is multilevel we use the numerical methods. The influence of the magnetic field on coherent population trapping effect for multilevel systems is considered. Some of our theoretical results coincide with known experimental ones.