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Journal of Physics B Atomic Molecular and Optical Physics

Relaxation study of electronic nuclear multipole moments through non-stationary Raman scattering of light in gas

A. I. Alekseev, V. N. Beloborodov, O. V. Zhemerdeev

Published Jan 14, 1989• 4 citations
Publisher

Abstract

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.

DOI
10.1088/0953-4075/22/1/016

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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.
A theoretical investigation of the non-stationary Raman scattering (RS) of light in gas atoms with no nuclear spin has been made. Account was taken of the level degeneracy due to the different orientation of the total angular momenta, the dependence of the RS signal on the polarisations of the light pulses and of the elastic depolarising collisions. Interesting RS polarisation properties have been found and assumed as a basis method for the identification of optically forbidden transitions and for the determination of parameters of the cubic susceptibility tensor. It has been proved that the polarisation properties and damping law of the non-stationary RS signal permit multipole relaxation rates of forbidden and allowed atomic transitions to be determined.
A method of determining relaxation rates of electronic and electronic nuclear multipole moments of gas atoms with non-zero nuclear spin, using the Stokes three-level echo (STE) and the photon echo (PE), has been proposed. This method utilises the polarisation properties and damping laws of the STE and PE on the inhomogeneously broadened transitions. Correct account was taken of the hyperfine structure (HFS) of the atomic levels and of the effect of the depolarising atomic collisions. The STE polarisation properties found have also been assumed to be a basis method for the identification of optically forbidden transitions in total angular momentum.
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.
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.
A theory is developed for the modified tri-level photon echo formed in gaseous media. Consideration is given to the cases when echo is generated both by atoms for molecules with zero nuclear spin and by atoms with non-zero nuclear spin. In the first case, it is shown that this particular kind of photon echo can be used to measure the relaxation characteristics of the multipole moments of the optically forbidden transition. On the basis of these considerations new experiments are suggested for the observation of the relaxation characteristics mentioned above. In the second case, formulae are obtained for the calculation of pre-exponential factors describing the dependence of the quantum beats of the intensity of the modified tri-level photon echo as a function of the time intervals between the exciting pulses. Values of the pre-exponential factors need to be known in order to correctly obtain spectroscopic information about an optically forbidden transition.
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.