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Physical Review A

Measurement of the recoil shift of saturation resonances of I2127 at 5145 Å: A test of accuracy for high-resolution saturation spectroscopy

Ch. J. Bordé, G. Camy, Bernard Decomps

Published Jul 1, 1979• 63 citations
Publisher

Abstract

We report the first observation of the recoil shift of an optical resonance in the visible part of the spectrum. The method rests on the fact that the recoil shifts have opposite signs for Doppler-generated level crossings with a common upper level and for those having a common lower level. The experiment has been performed with the argon laser at 5145 \AA{} as the source and iodine as the absorber. The measured values are within 12% of the theoretical recoil shift. We give a detailed discussion of the possible influence of shifts of various origins and especially light shifts on the measured frequency differences. We display saturated absorption and saturated dispersion spectra and give formulas for the intensities of the various resonances derived from the corresponding density-matrix diagrams.

DOI
10.1103/physreva.20.254

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Applied Physics Letters•Nov 1, 1981•331 citations
We report the first observation of the recoil shift of an optical resonance in the visible part of the spectrum. The method rests on the fact that the recoil shifts have opposite signs for Doppler-generated level crossings with a common upper level and for those having a common lower level. The experiment has been performed with the argon laser at 5145 \AA{} as the source and iodine as the absorber. The measured values are within 12% of the theoretical recoil shift. We give a detailed discussion of the possible influence of shifts of various origins and especially light shifts on the measured frequency differences. We display saturated absorption and saturated dispersion spectra and give formulas for the intensities of the various resonances derived from the corresponding density-matrix diagrams.
A theory is presented for the intensities of hyperfine components in saturation spectroscopy. We use a diagrammatic approach to nonlinear processes to derive closed-form formulas for the intensities of recoil doublets and of Doppler-generated level crossings. We discuss the influence of the terms introduced by hyperfine coherences in saturation spectroscopy. We also demonstrate spectroscopic stability when the hyperfine splittings are negligible. A catalog of simple formulas is given in view of applications to current spectroscopy and is illustrated by recent examples, including Doppler-free polarization spectroscopy. The extension to other sub-Doppler techniques such as two-photon Doppler-free spectroscopy is outlined. I.
The atomic-recoil effect leads to large (25%) asymmetries in a nearly ideal form of saturation spectroscopy based on Ca atoms that have been laser-cooled to . Starting with spectra from the more familiar Doppler-broadened domain, we show how the fundamental asymmetry between absorption and stimulated emission of light manifests itself when shorter spectroscopic pulses lead to the Fourier transform regime. These effects occur on frequency scales much larger than the size of the recoil shift itself, and have not been described before in saturation spectroscopy. These results directly impact precision spectroscopic measurements.
The commonly quoted saturation intensity of rubidium (Rb) for D2 transitions is 16.7W.m−2\mathrm{W}.\mathrm{m}^{-2}W.m−2. This value, however, is only accurate for the cycling transition, which renders the Rb atom to resemble a two-level system. In practice, the effective saturation intensity is influenced by various factors, such as the polarization of light, optical pumping, and atom collision which can redistribute the population. As a result, it is crucial to experimentally determine the effective saturation intensity. In this context, we demonstrate a novel yet simple experimental method to measure the effective saturation intensities of Doppler-broadened transitions in atomic vapours. Our method only requires on-resonance absorbance data for various input laser intensities, which can be obtained with a tunable CW laser without the need for precise frequency locking. We applied this method to measure the effective saturation intensities of all four Doppler-broadened D2 transitions in natural rubidium (Rb) vapour (27.8%87Rb and 72.2 %85Rb{}^{\text{8}} {}^{\text{5}}Rb85Rb) atr=35∘Cr={35}^{\circ} \mathrm{C}r=35∘C. The results show that the effective saturation intensities for Rb range from 0.752 to 16.8W.m−2\mathrm{W}.\mathrm{m}^{-2}W.m−2. Notably, for certain transitions (specifically, repump transitions), the effective saturation intensities were smaller than 16.7 W.m−2\mathrm{m}^{-2}m−2(up to an order of magnitude), with potentially important implications for optical pumping in Doppler-broadened transitions.
We analyze the excitation by an electromagnetic wave of a two-level molecule (or atom) within a rarefied gas. This process differs from the excitation of an isolated molecule because there is significant interaction between the molecule and the surrounding gas particles as they are all polarized by the electromagnetic wave. These interactions lead to corrections to the recoil and Doppler shifts of the molecule's transition frequency. We propose an experiment using saturation spectroscopy to observe sodium molecular transitions near the atomic DDD lines which could easily detect the correction to the first-order Doppler shift caused by the interaction between the sodium molecules and the surrounding atomic vapor.
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.