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Soviet Journal of Quantum Electronics

Spectral properties of resonant four-photon parametric oscillation

G. M. Barykinsky, Vladimir V. Lebedev, V M Plyasulya

Published Mar 31, 1982• 3 citations
Publisher

Abstract

An investigation was made of the spectral properties of four-photon parametric oscillation when the frequency of the generated field is tunable near an atomic resonance line. An ω4 = ω1–ω2+ω3 generation process involving coherent anti-Stokes scattering in thallium vapor was achieved experimentally. Biharmonic pumping was provided by resonant excitation of a 6P1/2–6P3/2 two-photon transition at the frequency ω1–ω2. Measurements were made of the oscillation power when the frequency ω3 was tunable near the frequency of a 6P3/2–7D3/2 transition at various thallium vapor pressures. It was found that the spectral properties of resonant parametric oscillation depend strongly on the concentration of active-mixture atoms and also on various saturation effects.

DOI
10.1070/qe1982v012n03abeh012174

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•May 10, 1996•2 citations
An investigation was made of the spectral properties of four-photon parametric oscillation when the frequency of the generated field is tunable near an atomic resonance line. An ω4 = ω1–ω2+ω3 generation process involving coherent anti-Stokes scattering in thallium vapor was achieved experimentally. Biharmonic pumping was provided by resonant excitation of a 6P1/2–6P3/2 two-photon transition at the frequency ω1–ω2. Measurements were made of the oscillation power when the frequency ω3 was tunable near the frequency of a 6P3/2–7D3/2 transition at various thallium vapor pressures. It was found that the spectral properties of resonant parametric oscillation depend strongly on the concentration of active-mixture atoms and also on various saturation effects.
An effort was made to optimize the coherent anti-Stokes scattering four-photon parametric oscillation process in thallium vapor in the 277 nm range. The dependence of the stimulated emission power on the thallium vapor pressure, confocal parameter, detuning from two-photon resonance, and pump power was investigated. The considerable saturation of the parametric oscillation power observed both with respect to the pump power and the vapor pressure was attributed to the breakdown of the wave interaction as a result of the strong high-frequency Kerr effect under two-photon resonance conditions.
An analysis is made of generation of the sum frequency ω3 = 2ω1 + ω2 in the case when the pump frequency coincides with that of a two-photon transition 2ω1 = ω21, and the frequency ω3 is tuned near the resonance line of an atom. Under conditions of resonance with the frequency of the generated field, the parametric process has some characteristic features associated with a strong competition between effects involving increases in the nonlinear susceptibility, absorption, and changes in the phase matching. Moreover, in the presence of a fairly high-intensity field due to a neighboring transition at the frequency ω2, a nonlinear Raman process (which changes the characteristics of the medium at the frequency ω3) begins to play an important part. It is found that the highest parametric oscillation powers over a wide spectral range may be achieved by appropriately varying the intensity of the field due to the neighboring transition, the atom concentration, or the interaction length.
An experimental investigation was made of the use of noise pumping in four-photon resonant parametric sum-frequency generation in potassium vapor. A two-photon resonance with the 9S1/2 and 7D3/2,5/2 levels and a one-photon resonance with the 10P1/2,3/2 and 11P1/2,3/2 levels were used. A comparison was made with the case of coherent pumping and it was found that, under conditions of strong dispersion and wave mismatch, the efficiency of the process using noise pumping differs negligibly from the efficiency using coherent pumping although the spectral density of the coherent pump is substantially higher than that of the noise pump.
Coherent radiation at several wavelengths in the vacuum ultraviolet (VUV) has been generated by four-wave parametric oscillation in mercury vapor. When a powerful ultraviolet pump laser of frequency omega(p) is tuned to a two-photon resonance, VUV signal photons at frequency omega(s), as well as idler photons at frequency omega(i), are generated such that omega(s) + omega(i) = 2omega(p). A frequency-doubled dye laser tuned to two-photon resonance with the 6s6d(1)D(2) level near 280.3 nm produced output at 184.9 and 143.5 nm. A tunable krypton fluoride excimer laser tuned to two-photon resonance with the 6s10s (1)S(0) level near 248.7 nm produced output at 140.1, 130.7, 130.1, 125.9, and 125.0 nm. Approximately 1-microJ, 200-W pulses were observed at 143.5 and 125.9 nm.
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.