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Journal of Physics B Atomic and Molecular Physics

Coherent anti-Stokes Raman scattering in caesium vapour

Alan Corney, K Gardner

Published Jun 14, 1978• 3 citations
Publisher

Abstract

Experiments are reported in which a pulsed dye-laser beam nu L was focused into a heat-pipe oven containing caesium vapour at densities of about 10 17 cm -3 . Optically pumped fixed-frequency infra-red laser emission nu IR and tunable stimulated electronic Raman-scattered radiation nu S were observed. In addition the generation of ultra-violet radiation by coherent anti-Stokes Raman scattering nu UV = nu L - nu S + nu IR was detected. Focused-beam phase matching appears to play a significant role in this process.

DOI
10.1088/0022-3700/11/11/020

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Journal of the Optical Society of America B•Mar 1, 1985•3 citations
Experiments are reported in which a pulsed dye-laser beam nu L was focused into a heat-pipe oven containing caesium vapour at densities of about 10 17 cm -3 . Optically pumped fixed-frequency infra-red laser emission nu IR and tunable stimulated electronic Raman-scattered radiation nu S were observed. In addition the generation of ultra-violet radiation by coherent anti-Stokes Raman scattering nu UV = nu L - nu S + nu IR was detected. Focused-beam phase matching appears to play a significant role in this process.
Experiments are reported in which a pulsed blue-dye laser beam ( omega L) was focused into a heat-pipe oven containing caesium vapour at densities of about 1023 cm-3. Tunable stimulated electronic Raman scattered infra-red radiation ( omega s) was observed together with radiation in the red region of the visible spectrum produced by optical frequency four-wave down conversion: omega R= omega L-2 omega s. Studies of the angular divergence and power of the red output beam demonstrate the importance of non-collinear phase matching in this process.
Stimulated electronic Raman scattering, SERS, is a simple method of efficiently generating widely tunable infrared radiation. This work describes techniques by which the tuning capability of this process may be extended. To this end several schemes in Caesium and Barium vapours have been investigated. In Barium vapour two Raman transitions were studied using fixed frequency lasers. Poor performance of one of these transitions led to the application of biharmonic pumping or 'coherent Raman mixing' to enable generation of infrared light, and was the first observation of this process in an atomic vapour. This technique was subsequently used to generate infrared light from tunable dye laser light, which gave continuous tuning from 1.16µm to 1.5µm. The process was found to be limited by atomic saturation. The effect which saturation has on the generation efficiency is considered theoretically, and predicts quite accurately the observed tuning behaviour. Two methods aimed at reducing molecular absorption effects in SERS in alkali vapours were investigated. The techniques employed either laser excitation and dissociation of the molecules or a reduction in their ground state concentration by superheating of the vapour. Some degree of success was achieved in improving the available tuning from the 6s-7s transition in Caesium. However, the inclusion of the effect of collision broadening of atomic transitions into a calculation of the Raman threshold suggests that little further improvement can be obtained on this transition. A direct measurement of the Raman threshold power on the 6s-5d5/2 transition in Caesium gave excellent agreement with theoretical predictions based on collision broadening of this Raman transition. In addition, this work gave an insight into the role photoionization plays in increasing the threshold under certain circumstances. The analysis suggests that laser pulse duration and vapour column length are important in determining whether Raman threshold can be exceeded.
The generation of 145.6-nm radiation by stimulated anti-Stokes Raman scattering in inverted atomic selenium was first reported by Ludewigt et al. 1 We have performed experimental studies of this process in similar excitation conditions, which allow us to compare some of the results in the two studies. The inverted population of the selenium (4p4)1S0 metastable state relative to the (4p4)3P0 state was prepared by photodissociation of COSe vapor using broadband 193-nm radiation from an ArF excimer laser. The pump beam at 205.1 nm was generated by the first-order Stokes shift in deuterium of narrowband (0.27-cm–1), 193-nm radiation from a separate, tunable ArF laser. The pump beam was tuned near the selenium (4p4)1S0–(4p35s)3P1 intermediate resonance to generate tunable, coherent radiation at 145.6 nm. We have studied the process in a variety of experimental conditions. Factors affecting the conversion efficiency and tunability include the initial COSe pressure, the intensities and relative timing of the photolyzing and pump beams, and the presence of buffer gases. The experimental results are compared with theoretical calculations based on a recently developed three-level model2 which incorporates Doppler broadening and arbitrary decay times.