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Topical Meeting on Laser Techniques in the Extreme Ultraviolet

Anti-Stokes Raman Lasers

J. C. White, D. Henderson

Published Jan 1, 1982• 1 citation
Publisher

Abstract

This paper reports what we believe to be the first observations of stimulated, anti-Stokes Raman laser emission. A metastable Tl*(6p 2po3/2) population inversion was created by selective photodissociation of TlCl, and Raman scattering using 532 nm and 355 nm pump lasers resulted in stimulated emission at 376 nm and 278 nm, respectively. Likewise, inverted I*(5p5 2Po1/2) atoms have been used as a Raman medium; and with a 206 nm pumping source, we have generated tunable VUV radiation at 178 nm.

DOI
10.1364/euvs.1982.mc2

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This paper reports what we believe to be the first observations of stimulated, anti-Stokes Raman laser emission. A metastable Tl*(6p 2po3/2) population inversion was created by selective photodissociation of TlCl, and Raman scattering using 532 nm and 355 nm pump lasers resulted in stimulated emission at 376 nm and 278 nm, respectively. Likewise, inverted I*(5p5 2Po1/2) atoms have been used as a Raman medium; and with a 206 nm pumping source, we have generated tunable VUV radiation at 178 nm.
The first observation of nonresonant, stimulated anti-Stokes Raman emission is reported. A metastable Tl(6p2P32o)\mathrm{Tl}(6p^{2}P_{\frac{3}{2}}^{o})Tl(6p2P23​o​) inversion is created by selective photodissociation of TlCl. Raman scattering from the Tl metastable state to ground using 532- and 355-nm pump lasers resulted in stimulated emission at 376 and 278 nm, respectively. Conversion efficiencies up to 10% are reported.
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
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.