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Le Journal de Physique Colloques

ANTI-STOKES RAMAN LASERS : A CONCEPT FOR THE GENERATION OF SHORT-WAVELENGTH COHERENT RADIATION

B. Wellegehausen, Klaus Ludewigt, M. HUBE, Alfred O. Feitisch

Published Dec 1, 1987• 2 citations
Publisher

Abstract

The anti-Stokes Raman process allows frequency up-conversion of coherent pulsed or cw radiation. For the process, a population inversion on a two-photon transition is needed. The principale of this technique, the present experimental situation and some developments will be described and discussed.
DOI
10.1051/jphyscol:1987778

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The anti-Stokes Raman laser process is an interesting method for frequency upconversion and generation of tunable UV radiation. This method requires no index matching and allows high-conversion efficiencies and output energies and large frequency shifts in a single step. A basic requirement is a population inversion between a metastable level and a suitable lower-lying level. So far anti- Stokes laser emission has been demonstrated using the metastable TI (6P3/2). l(5P1/2). and Br (4P1/2) levels, where a population inversion with respect to the corresponding atomic ground states has been generated by photodissociation of suitable compounds.1-3 For the Tl system efficiencies of 10 % and output energies of ~1 mJ (at 377 nm) have been reported,1 and with Br a shortest wavelength of 149 nm was possible by upconversion of 157.5-nm radiation of a F2 laser.3
A new process capable of scattering intense anti-Stokes waves that uses stimulated electronic Raman scattering in metal vapor is proposed. The coherent material excitation produced by a prepump pulse couples with the forthcoming main pulse exclusively to create polarization that radiates the anti-Stokes wave. The selection rule governed by angular momentum conservation is the key to cause such strong coupling to induce unidirectional upconversion without any population inversion. The power conversion efficiency from the pump wave to the anti-Stokes wave is theoretically expected to reach 100% in this process.
We experimentally demonstrate efficient Raman conversion to respective Stokes and anti-Stokes fields in both pulsed and continuous modes with a Rb-87 atomic vapor cell. The conversion efficiency is about 40-50% for the Stokes field and 20-30% for the anti-Stokes field, respectively. This efficient conversion process is realized with coherent feedback of both the Raman pump and the frequency-converted fields (Stokes or anti-Stokes). The experimental setup is simple and can be applied easily to produce light sources with larger frequency shifts using other Raman media with long coherence time. They may have potential applications in nonlinear optics, Raman spectroscopy and precision measurement.
We propose to use population stored in the radiatively trapped 6°P1° atomic mercury resonant level (1850 Å) for frequency conversion by an anti-Stokes or two-photon process. Inversion is with respect to the lower-lying 63P °0,1,2 levels which are assumed empty following selective quenching or rapid conversion to the mercury dimer. Photon conversion gains of 2.5×10−2 cm/MW for 1.06-μm and 8.7×10−5 cm/MW for 10.6-μm input wavelengths with corresponding 0.4157- and 0.9116-μm output wavelengths are calculated at a 1016-cm−3 inversion density.
Coupled differential equations are formulated to model the generation of coherent anti-Stokes Raman radiation in molecular gases. They include the basic coherent interaction of incident pump and idler (Stokes) waves to generate the anti-Stokes radiation plus other radiation and absorption processes which influence saturation due to population depletion of the lowest energy level. Other factors considered are simultaneous excitation of more than one vibration frequency, a quasi-monochromatic idler beam slightly off the true Stokes frequency, and the temporal laser pulse shape. Some effects of these various physical factors on saturation are presented graphically.