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Journal of Physics B Atomic and Molecular Physics

Effects of spin-orbit coupling on resonant enhancement of stimulated electron Raman scattering

D. Cotter, D.C. Hanna

Published Sep 11, 1976• 20 citations
Publisher

Abstract

The resonant enhancement and polarization properties of stimulated electronic Raman scattering by alkali metal atoms are investigated. Spin-orbit splitting of nearly-resonant intermediate levels results in 90 degrees rotation of the plane of polarization of the stimulated Stokes radiation. The relationship to two-photon absorption is also described.

DOI
10.1088/0022-3700/9/13/005

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The resonant enhancement and polarization properties of stimulated electronic Raman scattering by alkali metal atoms are investigated. Spin-orbit splitting of nearly-resonant intermediate levels results in 90 degrees rotation of the plane of polarization of the stimulated Stokes radiation. The relationship to two-photon absorption is also described.
The main properties of infrared stimulated electronic Raman scattering (SERS) at the 6 2 S 1/2 -7 2 S 1/2, 3/2 transitions in cesium atoms are studied theoretically and experimentally as functions of the atomic concentration, which was varied from 10 11 to 10 16 cm −3 . It is found that the efficiency of generation of Stokes radiation strongly depends on one-photon absorption of the pump radiation tuned near frequencies of the 6 2 S 1/2 -7 2 P 1/2, 3/2 transitions. By using the equation for the density matrix, which describes the evolution of a three-level system, the theory of resonance excitation of IR radiation upon one-photon absorption at an adjacent transition is developed. The theory describes well the main features of IR SERS in alkali-metal vapors.
An enhanced two-photon emission has been observed between the 6S and the 4S levels of potassium. The priming field is the stimulated electronic Raman emission at 2720 cm-1due to scattering of ruby laser radiation from the4P_{3/2}state in potassium. The intense emission at the complementary frequency ω2is close to the 5P → 4S resonance lines. As a result, the coupling coefficient has a resonance character that is favorable for the enhancement. The observed results are compared with a simple analysis. The relation of the enhanced emission with two-quantum absorption, stimulated Raman effect, and parametric four-photon processes is discussed.
A report is given of the first quantitative study of the spontaneous and stimulated electronic Raman scattering by a resonance doublet of the sodium atom excited resonantly at the D 1 and D 2 lines by a tunable dye laser. Theoretical and experimental analyses of the differential scattering cross section and polarization properties at the Stokes and anti-Stokes frequencies show that the observed scattering is due to a nearly resonant process involving the ground state 3 S 1/2 as the dominant intermediate state. The stimulated Stokes and anti-Stokes scattering lines, which are shifted from the D 1 and D 2 lines by an amount corresponding to the frequency separation between lowest-lying excited doublets 3 P 1/2 and 3 P 3/2 , are observed by exciting a sodium vapor cell with a passively mode-locked dye laser.
A theory is developed for the calculation of the gain g due to stimulated resonant hyper-Raman scattering of light by polaritons in gaseous media. It is shown that throughout the tuning range of the pump frequency (including one- and two-photon resonances) a maximum of g corresponds to a dispersion curve of polaritons plotted ignoring attenuation. Theoretical results are used to analyze characteristics of hyper-Raman scattering in sodium vapor. It is shown that under normal experimental conditions the splitting of polariton branches is considerable (amounting to tens of reciprocal centimeters on the frequency scale and several angular degrees). The value of g is estimated for two-photon resonances in the case when the pump frequency is tunable in a wide range. The optimal conditions for stimulated hyper-Raman scattering are identified.