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Journal of Applied Spectroscopy

Unsteady-state four-photon parametric interaction of time-spaced waves in a Raman-resonance medium

G. V. Arutyunyan, G. P. Dzhotyan

Published Feb 1, 1986• 0 citations
Publisher
DOI
10.1007/bf00660364

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Soviet Journal of Quantum Electronics•Jul 31, 1985•8 citations
The collinear generation of radiation with a multicomponent spectrum is obtained upon scattering of picosecond pulses in gaseous hydrogen coherently excited by the pulsed biharmonic pump in resonance with the Raman-active rotational S 0 (1) transition. Probe pulses at 355 nm were almost completely transformed to the radiation with the multicomponent spectrum of width ~5000 cm -1 and the components spaced by 587 cm -1 . The solution of a system of equations for the four-photon Raman — parametric interaction is obtained in the plane-wave dispersionless approximation in the spectral and time representations. The equations describe the transformation of probe pulses in gas with the induced coherence into an arbitrary number of interacting spectral components. The consideration performed in the second order of the dispersion theory provides good agreement with experiments on the transformation into different spectral components depending on the probe-pulse delay.
A theoretical investigation is made of unsteady quasiresonant optical third-harmonic generation in a gaseous nonlinear medium pumped by amplitude-modulated pulses of constant collimated radiation. It is shown that two effective unsteadiness mechanisms exist: wave unsteadiness, associated with the difference between the propagation velocities of the pump and harmonic waves, and local unsteadiness caused by the finite relaxation time of the appropriate nonlinear component of the polarization of the medium. In spectral terms these correspond to the resonant dispersion of the phase matching and the dispersion of the nonlinear polarizability of the medium, respectively. The output pulse profile is determined and the influence of the main parameters on its profile is analyzed. The stimulated emission spectrum is also studied for conditions when the pump field is a steady-state random Gaussian process.
Investigations are made of hyper-Raman scattering and four-photon parametric processes in two-photon excitation of metal vapor. The laws of propagation of infrared and ultraviolet radiation generated in a metal vapor medium by these processes are found for the steady-state interaction. The nonlinear polarization of the medium is obtained in terms of elements of the atomic density matrix allowing for saturation by the pump field and for the influence of collisions. The spectral and tuning characteristics of the converted radiation are studied and a comparison is made with experimental data. A dip observed in the infrared radiation spectrum for hyper-Raman scattering and its broadening are explained. A detailed discussion is given of the role of collisions that substantially narrow the tuning range of the infrared radiation in hyper-Raman scattering.