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Physical Review A

Saturation spectroscopy with laser optical pumping in atomic barium

P. G. Pappas, Michael M. Burns, David D. Hinshelwood, Michael S. Feld, Daniel E. Murnick

Published Jun 1, 1980• 181 citations
Publisher

Abstract

The magnitude and sign of laser saturation resonances induced in atomic transitions with level degeneracy can be dramatically altered by the presence of optical pumping. This paper presents a detailed theoretical treatment of optical-pumping Lamb dips and crossover resonances, and their experimental observation in the 553-nm barium resonance transition. The physical principles underlying the laser optical-pumping saturation effect are also discussed.

DOI
10.1103/physreva.21.1955

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arXiv:0808.1272•Physical Review A•Oct 14, 2008•1 citation
The magnitude and sign of laser saturation resonances induced in atomic transitions with level degeneracy can be dramatically altered by the presence of optical pumping. This paper presents a detailed theoretical treatment of optical-pumping Lamb dips and crossover resonances, and their experimental observation in the 553-nm barium resonance transition. The physical principles underlying the laser optical-pumping saturation effect are also discussed.
We have studied the effects of optical pumping and near-resonant radiation pressure that compete with the saturation effect on the formation of the line shapes of Doppler-free saturation absorption spectra of alkali atoms. We have measured the reverse of the sign of F g =3 to F e =4 saturated absorption of the rubidium D 2 line and the change in its asymmetry as the optical pumping effect is gradually turned on compared with the saturation effect. The experimentally observed behaviors of optically pumped Lamb dips and crossover resonances in rubidium show good agreement with the calculation using the phenomenological model previously introduced for cesium.
The behaviour of an optically thick column of barium vapour resonantly 10 -2 illuminated at 553.5m by a 50 ns, 10 Wm pulse from a flashlamp pumped dye 19 21 -3 laser system was investigated for barium number densities in the range 10 -10 m in the presence of He buffer gas at 100 Torr.A variety of optical saturation effects associated with the principal resonance transition were studied.In marked contrast to earlier work, saturation of the intensity of the scattered light near 553.5 nm with increasing laser power was found for a suitable geometry of the collection optics but at a laser intensity typically two orders of magnitude higher than that predicted by simple theory, despite the fact that this theory was found to describe correctly transmission measurements along the length of the vapour column.The apparent contradiction between the fluorescence and transmission results, which indicated that the scattered radiation intensity continued to rise with incident laser power, despite the population of the upper resonance level having reached a limiting saturation value, could be understood in terms of a simple model which took into consideration the spectral distribution of the scattered light and its transfer through the unexcited vapour.However, in common with other similar experiments, saturation of the scattered radiation intensity with laser power could not be totally achieved when a more usual collection optics geometry was employed.This was interpreted as a consequence of laser intensity variation across the face of the laser beam.A number of subsidiary experiments were performed.These included spatially resolved intensity measurements of the scattered radiation and time resolved metastable level population measurements.In addition, evidence for laser induced ionization was sought using two different methods and this enabled an upper limit of 10% ionization to be placed on the experiments in the present work.
A theory of saturation spectroscopy is developed which accounts for effects of level degeneracy. The theory can be applied to those situations in which a pump laser field of arbitrary strength and polarization acts between two manifolds of degenerate or nearly degenerate atomic levels, while a probe laser field of arbitrary strength and polarization acts between a coupled manifold of levels. As such, this theory of "three-level" systems could, in principle, include effects arising from level degeneracy, optical pumping, atomic motion, transient laser fields, different polarizations and strengths for pump and probe fields, and atomic transit across the laser fields. The present calculation, however, is limited to a study of optical pumping and field polarization effects for pump fields of arbitrary strength and weak probe fields interacting with a single velocity subclass of atoms. Probe absorption line shapes clearly display the effects of pump-field strength (Rabi splittings), pump-field polarization (positions and number of Rabi-split resonance peaks), pump-field detuning (positions of resonance peaks), and optical pumping (relative strengths of the resonance peaks). The calculation is carried out with the use of an irreducible tensor basis for the atomic density matrix although a standard (mmm-basis) calculation is included in an appendix.
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.
The recoil effects of spontaneous photon emissions during optical pumping of a trapped three-level atom are exactly calculated. Without resort to the Lamb-Dicke approximation, and considering arbitrary detuning and saturation of the pump laser, the density of recoil shifts in phase space is derived. It is shown that this density is not of Gaussian shape, and that it becomes isotropic in phase space only for a branching ratio corresponding to fluorescence scattering but unfavorable for optical pumping. The dependence of its anisotropy on the laser saturation is discussed in the resonant case, and the mapping of moments of the atom's center-of-mass motion due to the pumping is presented. Moreover, it is shown how optimum parameters for protecting the center-of-mass quantum state from pump-induced disturbance depend on the specific property to be protected.