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Journal of Physics B Atomic Molecular and Optical Physics

Optical activity in the observation of quantum beats in forward scattered light

K. Szymaniec, J. Koperski, S.N. Lea, T. Dohnalik

Published Jul 28, 1995• 1 citation
Publisher

Abstract

The technique of quantum beats in forward scattering remains a useful tool for atomic and molecular spectroscopy. The detected signal is strongly dependent on experimental conditions such as the dichroism and birefringence of external optical elements. We present a theoretical model and its experimental verification to give a physical insight into these effects.

DOI
10.1088/0953-4075/28/14/011

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The technique of quantum beats in forward scattering remains a useful tool for atomic and molecular spectroscopy. The detected signal is strongly dependent on experimental conditions such as the dichroism and birefringence of external optical elements. We present a theoretical model and its experimental verification to give a physical insight into these effects.
The optical magnetic birefringence (Faraday) technique that can be used to study the anisotropy distributions of the angular momenta of photofragments produced in molecular photodissociation is compared theoretically and experimentally with the magnetic dichroism technique. The frame independent tensor form of the general expression describing the difference between an initial and a final polarization matrix of a probe light beam passing through the photofragment vapor is presented and analyzed. The procedure of detection of the photofragment electron orientation and alignment angular distributions by Doppler spectroscopy using each of the techniques is studied theoretically. The angular independent anisotropy orientation and alignment parameters describing photodissociation dynamics that can be determined from these studies are presented. It is shown that in principle each of the techniques can give the same information about the photodissociation dynamics; however, the birefringence technique has an undeniable advantage since it leads to an increase in accuracy of the experimental data. Both magnetic birefringence and magnetic dichroism techniques were used experimentally to study the spin orientation of ground state Rb atoms produced in photodissociation of RbI at 266 nm by circularly polarized laser light. The experiment was not of the Doppler spectroscopy type, but use of different 85 Rb and 87 Rb isotopes in the dissociation cell and in the probe light source allows detection of the oriented atomic photofragments separately by each of the techniques. Obtained experimental results are in agreement with the theoretical predictions. Contribution of the orientation of the Rb hyperfine structure energy states to the observed signals were also studied and treated theoretically. The initial degree of the electron spin orientation of the Rb atoms produced in the reaction was found to be P e = 0.11 ± 0.02.
Previous theoretical treatments of polarisation spectroscopy (forward scattering) are generalised so as to include laser temporal coherence effects. It is shown that for the general case it is impossible to describe the signal obtained in terms of birefringence and dichroism. The generalisation of the concept of the polarisability tensor is given together with the approximate expression for the signal in terms of it. The simple example of the J g =0 to J e =1 transition in the forward scattering experiment is discussed in detail. Comparison is made between the signal lineshapes obtained for the phase diffusion model and the chaotic field model. The necessity of taking into account the statistical properties of the laser light in the forward scattering (polarisation spectroscopy) experiment is pointed out.
A theoretical study of the polarization dependence of stimulated Rayleigh-wing scattering and the optical-frequency Kerr effect has been undertaken. When the incident light is circularly polarized, a striking difference in gain is found for the co- and counter-rotating senses of polarization of the scattered light---the former being suppressed and the latter being exceptionally favored. The analysis begins with a model for the Kerr effect, which involves the alignment of anisotropic molecules in an electric field, but the results can be immediately generalized to any light scattering process of tensor symmetry. The nonlinear problem of the propagation of an intense elliptically polarized light wave in a Kerr-active medium is shown to have a solution in which the vibrational ellipse undergoes self-precession and self-retardation. The stimulated scatterings or instabilities of such a self-precessing and self-retarding light wave are obtained for the backward and forward directions. Birefringence, optical activity, and linear and circular dichroisms are some of the phenomena which result, but the forward direction yields substantially different results from the backward direction because of Stokes-anti-Stokes coupling.