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Soviet Journal of Quantum Electronics

Transient coherent Doppler-free spectroscopy of two-photon absorption in the presence of depolarizing collisions

Aleksey I. Alekseev, V. N. Beloborodov

Published Aug 31, 1992• 0 citations
Publisher

Abstract

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.

DOI
10.1070/qe1992v022n08abeh003593

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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.
The Raman photon echo (RPE) in atomic vapour, allowing for depolarising atomic collisions and hyperfine structure of the atomic levels, has been studied theoretically. A new method of determining the electronic and electronic nuclear relaxation rates of the multipole moments of gas atoms with nonzero nuclear spin using the RPE has been proposed. The RPE method also makes it possible to measure the derivatives of these relaxation rates with respect to the impurity gas pressure. A method of determining the energy separation between the hyperfine structure sublevels has been developed. This method is based on the quantum beats of the RPE intensity and may be used when the hyperfine splitting is less than the Doppler linewidth. A possibility of identifying the forbidden transitions in both the electronic and total angular momenta has been shown.
A method of determining the relaxation constants of the multipole moments of gas atoms with non-zero nuclear spin has been proposed by using the polarisation properties and damping law of the non-stationary Raman scattering (NRS) of light. Correct account was taken of the depolarising atomic collisions and of the effect of the hyperfine structure (HFS) of the atomic levels. The NRS polarisation properties found have been assumed to be a basis method for the identification of optically forbidden transitions in both the electronic and total angular momenta. A possible method of determining the HFS constants through analysis of the NRS quantum beats has been established.
Method of stimulated photon echo with specially chosen linear polarizations of exciting pulses of coherent resonant radiation is applied for investigation of collisional decay of orientation and alignment in molecular gas SF6 and its mixtures with buffers He and Xe. These relaxation rates are measured as a function of longitudinal velocities. Within experiment accuracy, no remarkable velocity dependence of depolarizing collisions rates was detected. This result confirms conventional approach of depolarizing collisions theoretical treatment.
Polarization nondegenerate nonstationary coherent anti-Stokes Raman spectroscopy was used in measurements of pulse responses for separate electronic multipole moments. The 6P(1/2)-6P(3/2) transition of Tl atoms was investigated. Doppler dephasing conditions, quantum beats of the hyperfine components of this transition are clearly seen when pure anisotropic scattering is registered, but they are small in the case of purely antisymmetric scattering. Under collisional dephasing conditions the relaxation rates of anisotropic and antisymmetric scattering agree with existing theory within +/-5%.