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Physical Review A

Anti-Stokes Raman lasers without inversion

Andrew J. Merriam, Alexei V. Sokolov

Published Jul 1, 1997• 6 citations
Publisher

Abstract

We describe the propagation dynamics and gain line shape of pulsed, tunable, anti-Stokes Raman lasers without inversion. Analytical expressions for the gain are obtained and evaluated for inhomogeneously broadened atomic media. The inversionless gain, which requires selective pumping of one of two lower atomic states, occurs regardless of the relative populations of these states and vanishes when the atomic populations are in equilibrium.

DOI
10.1103/physreva.56.967

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We describe the propagation dynamics and gain line shape of pulsed, tunable, anti-Stokes Raman lasers without inversion. Analytical expressions for the gain are obtained and evaluated for inhomogeneously broadened atomic media. The inversionless gain, which requires selective pumping of one of two lower atomic states, occurs regardless of the relative populations of these states and vanishes when the atomic populations are in equilibrium.
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
Nonresonant stimulated anti-Stokes Raman scattering from an inverted population in atomic iodine has been observed. The population inversion was achieved by flash photolysis of trifluoromethyliodide. A gain of e7{e}^{7}e7 was measured for a laser probe pulse at the anti-Stokes wavelength passing through the inverted iodine coincident with a laser pump pulse. This result is in good agreement with theoretical predictions.
Threshold characteristics for an anti-Stokes Raman laser based on inverted, metastable TI * (6p(2)P degrees (3/2)) atoms are studied. Raman upconversion of a tunable dye laser at 535 to 378 nm is observed with an overall tuning range of 1125 cm(-1) for a single-pass laser device. The anti-Stokes pump-laser threshold varies inversely as the square of the detuning from the intermediate Raman level, except in a region ~50 cm(-1) to either side of the resonance, where the threshold is constant. These observations are explained in terms of group-velocity dispersion effects and are in good agreement with a simple theoretical model.
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.