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Journal of Applied Spectroscopy

Theory of four-photon scattering in conditions of intense resonant excitation

Sergey K. Potapov, Vladimir Leonardovich Derbov, A. F. Bukatin

Published Jan 1, 1985• 1 citation
Publisher
DOI
10.1007/bf00661118

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An analysis was made of four-photon interaction processes under conditions of two-photon resonance excitation of the 3 D sodium level by two-frequency radiation from a single-pulse picosecond YAG:Nd laser with frequency doubling and a KDP optical parametric oscillator. The spatial and frequency spectra of the four-photon parametric scattering (FPPS) were recorded and studied experimentally at various sodium vapor densities (10 15 –10 17 cm −3 ) and also using collinear and noncollinear excitation. It was found that the observed conical structure of the FPPS radiation may be interpreted by an analysis of whether the frequency and spatial phase-matching conditions were satisfied. Dependences of the intensity of the FPPS radiation on the intensity of the exciting radiation, the sodium vapor density, and the detuning of the exciting radiation frequency from the two-photon resonance were obtained.
Coherent four-photon scattering of light due to excited and autoionizing states of atomic systems is considered. We analyze the influence of one-photon resonances at the frequency of the anti-Stokes signal and at the frequency of the pump wave on the shape of the spectrum of four-photon scattering. We derive analytical expressions for the line shapes of four-photon scattering involving one-photon resonances with allowance for phase-matching conditions and variation in the populations of excited states for limiting regimes of tight focusing and strong absorption in a medium with a cubic nonlinearity. The calculated spectra of four-photon scattering include the interference of resonant and nonresonant components of the third-order nonlinear susceptibility with allowance for one-photon saturation. We develop a method for normalizing experimental spectra of four-photon scattering with one-photon resonances that takes into account distortion of spectral lines due to the influence of phase mismatch and one- photon absorption.