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Journal of Physics B Atomic and Molecular Physics

Observations of stimulated anti-Stokes radiation in barium vapour

John L. Carlsten, Thomas J. Mcilrath

Published Apr 1, 1973• 8 citations
Publisher

Abstract

Stimulated anti-Stokes emission at 457.6 nm accompanying the transition from the 3 D 2 metastable to the 1 S 0 ground state in barium has been observed when the output of a dye laser is tuned close to the intercombination line at 791.1 nm. The emission is interpreted as parametric four-wave coupling. Scattering at other frequencies is also observed and the possibility of using this process to produce tunable ultraviolet light is briefly discussed.

DOI
10.1088/0022-3700/6/4/009

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Stimulated anti-Stokes emission at 457.6 nm accompanying the transition from the 3 D 2 metastable to the 1 S 0 ground state in barium has been observed when the output of a dye laser is tuned close to the intercombination line at 791.1 nm. The emission is interpreted as parametric four-wave coupling. Scattering at other frequencies is also observed and the possibility of using this process to produce tunable ultraviolet light is briefly discussed.
Two-photon resonant or nearly resonant optical processes have been investigated in atomic barium vapour ( approximately 10 17 cm -3 ) with a pulse dye laser (frequency omega L ) covering the range 735-415 nm. These interactions result in strong coherent emissions emitted either forward and backward, or forward only. The optical processes responsible for these coherent emissions have been identified. Seventy five lines (frequency omega ES ) emitted from 1000 to 360 nm are due to optically pumped stimulated emissions or stimulated electronic hyper-Raman scattering. Twenty eight lines (frequency omega sigma ) observed from 795 to 250 nm are generated through four-wave-mixing parametric processes with omega sigma =2 omega L +or- omega ES , and nine- (795-260 nm) through six-wave-mixing parametric processes with omega sigma =2 omega L - omega ES1 - omega ES2 +or- omega ES3 .
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 phosphate neodymium glass laser emitting picosecond pulses tunable in the 1.05–1.07 μ range was developed to study nonlinear optical processes in atomic barium vapor. Its temporal characteristics were investigated using a modified second harmonic beam method. Electron stimulated Raman scattering and four-photon parametric conversion in atomic barium vapor were used to obtain efficient conversion of the third harmonic of the picosecond phosphate laser (350–356 nm) to the Stokes (580–600 nm) and anti-Stokes (250–253 nm) waves. The highest conversion quantum efficiency for the Stokes wave was 15%. Electron stimulated Raman scattering in an (6 s 2 ) 1 S –(6 s 7 s ) 1 S –(6 s 6 p ) 1 P 0 system, having a strongly forbidden first transition, was recorded for the first time. In the same system, two-photon pumping generated four-photon parametric superradiance and it was found that the signal and idler waves had anomalously broad spectra (wider than 100 cm −1 ).
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.