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Journal de physique

Two Photon Polarization Spectroscopy

V.Paul Kaftandjian, B. Talin, Lewis S. Klein

Published Jan 1, 1979• 8 citations
Publisher

Abstract

Dichroism and birefringence are studied for the case of a strong saturating laser and a linearly polarized weak probe laser interacting with a dilute gas. For linearly or circularly polarized saturating laser fields the optical analog of the Kerr or Faraday effect are obtained respectively. Two photon, Doppler-free polarization effects are studied for two and three level systems (J = 0 → J = 1 and J = 0 → J = 1 → J = 0). The transition from the Autler-Townes effect conditions to those of the Lamb-dip is examined as a function of the system Doppler width.

DOI
10.1051/jphys:0197900400110103700

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Dichroism and birefringence are studied for the case of a strong saturating laser and a linearly polarized weak probe laser interacting with a dilute gas. For linearly or circularly polarized saturating laser fields the optical analog of the Kerr or Faraday effect are obtained respectively. Two photon, Doppler-free polarization effects are studied for two and three level systems (J = 0 → J = 1 and J = 0 → J = 1 → J = 0). The transition from the Autler-Townes effect conditions to those of the Lamb-dip is examined as a function of the system Doppler width.
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.
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.
A previously developed diagrammatic method for calculating the nonlinear response of a dilute gas at near resonance with strong classical radiation fields is extended to include velocity-dependent homogeneous and inhomogeneous broadening phenomena. The method is applied to two-level saturated-absorption (Lamb-dip) spectroscopy. Expressions are obtained for the collision-broadened Lamb dip probed by a weak field in the presence of an arbitrarily strong saturating field and are compared to the usual infinite-Doppler-width, weak-saturation expression. We study the effects of velocity and momentum transfer on the line-shape parameters and discuss the effect of phase-changing and strong inelastic collisions on the intensity.
We demonstrate polarization spectroscopy of an excited state transition in room-temperature cesium vapor. An anisotropy induced by a circularly polarized pump beam on the D2 transition is observed using a weak probe on the 6P(3/2)→7S(1/2) transition. At high pump power, a subfeature due to Autler-Townes splitting is observed that theoretical modeling shows is enhanced by Doppler averaging. Polarization spectroscopy provides a simple modulation-free signal suitable for laser frequency stabilization to excited state transitions.