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Polarization four-photon spectroscopy with elliptically polarized and completely unpolarized light

Igor I. Gancheryonok, Inna V. Gaisyonok

Published May 8, 1994• 0 citations
OpenAlex

Abstract

When intense radiation (pumping) passes through a resonant medium, a change in polarization of another (probe) beam can take place. A pump wave induces optical anisotropy in an initially isotropic medium, which leads to dichroism and birefringence. Many papers have been concerned with the effect of resonant changes of the probe polarization slate; however, in most of these papers the authors have been limited by simplified cases with linearly or circularly polarized interacting beams.

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When intense radiation (pumping) passes through a resonant medium, a change in polarization of another (probe) beam can take place. A pump wave induces optical anisotropy in an initially isotropic medium, which leads to dichroism and birefringence. Many papers have been concerned with the effect of resonant changes of the probe polarization slate; however, in most of these papers the authors have been limited by simplified cases with linearly or circularly polarized interacting beams.
A theoretical investigation of the change in polarization of ultrashort pulses of light near the two-photon resonance is carried out. A strong wave of circular polarization in the medium induces optical anisotropy which affects the change in weak probe-wave polarization. It is shown, that owing to an interaction transient, the probe-wave polarization becomes elliptical whose parameters change depending on time and position. This leads, in turn, to oscillation dependence of the rotated component of the probe field amplitude on the pumping energy, and the length and density of the resonant medium.
Abstract Based on the light-induced polarization ellipse rotation effect, we propose an optical Kerr gate (OKG) in which elliptically polarized probe light is used by introducing a pair of crossed quarter-wave plates into the conventional OKG arrangement, placed just before and after the Kerr medium. Transient birefringence induced by the pump beam in the Kerr medium leads to a rotation of the polarization ellipse of the probe beam, hence part of the probe beam would pass through the OKG. Theoretical calculations and experimental results both indicate that the OKG signal intensity would reach the optimum value independent of the pump polarization direction when the probe beam is circularly polarized. This modified OKG measurement is suitable to detect the third-order nonlinearities induced in anisotropic materials.
The optical-pumping theory of the passage of polarised radiation through a resonant medium was developed in the irreducible tensorial formalism. Transitions with arbitrary momenta J 1.2 are considered in the cubic approximation. For transitions with small values of momenta (J 1 =1 to J 2 =0; J 1 = 1 / 2 to J 2 = 1 / 2 ) the vector form of the equation system in density-matrix notation allows the problem to be solved exactly for light intensity. In the general case of an elliptically polarised wave, the equation systems for the interaction between circular components of polarisation of light in a resonant medium are obtained. Numerical calculations for deformation and rotation of the polarisation ellipse in a medium subject to saturation effects are also carried out. Irrespective of the initial state the polarisation tends either to a linear or to a circular form as it propagates, depending on times of collisional relaxation of orientation and alignment. The polarisation of linearly and circularly polarised waves does not change as the waves propagate, but the values of the saturation power for these polarisations differ considerably.
A theoretical analysis of the relative intensities of the Doppler-free signals in saturation spectroscopy, velocity selective optical pumping (VSOP) spectroscopy, polarization spectroscopy and a mixing of saturation and polarization spectroscopies is presented using the approximation of a single cycle of optical pumping in a four-level system. An optical pumping process in the Zeeman sublevels is taken into account owing to the important role of spontaneous emission even if the sublevels are degenerate. Arbitrary polarization combinations are considered for pump and probe beams. The similarities and differences between three kinds of spectroscopy are made clear. Both circular and linear optical anisotropies induced by the pump beam are considered in this theoretical calculation. The magnitude and sign of Doppler-free resonances in each spectroscopy are quite different owing to the polarizations of the pump and probe beams. The four-level system is important as a three-level approximation. The results obtained from the four-level optical pumping theory are in good agreement with experimental reports.
We have observed the Doppler-free dichroism and birefringence induced by a linearly polarized laser beam (pump beam) by monitoring the polarization and amplitude changes of a weak probe beam through an analyzer. The effects have been observed in two-level systems and also in three-level systems of Ne I. At rather low pump power, a typical refractive-index anisotropy of 10−8 has been measured. We have shown that, when the normal resonance curve exhibits a broad background due to collisions, our method allows the elimination of this background. In addition, using a rotating analyzer, we have obtained simultaneously the dichroism and birefringence curves, i.e., the imaginary and real part of the anisotropic-induced susceptibility.