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Soviet Journal of Quantum Electronics

Four-photon parametric oscillation in thallium vapor

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

Published Mar 31, 1979• 0 citations
Publisher

Abstract

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.

DOI
10.1070/qe1979v009n03abeh008888

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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 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.
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.
The nonlinear response of sodium vapor with a laser tuned near the 4D two-photon resonance is investigated over a large range of sodium concentrations and pump intensities with emphasis on the influence of coherent cancellation effects on the induced polarizations and the primary mechanism for the generation of the new frequencies. Over a wide range of circumstances, the response of the medium is dominated by parametric four-wave mixing as compared to amplified spontaneous emission or stimulated electronic hyper-Raman scattering. Secondary four-wave-mixing fields are generated by stimulated Raman scattering of one parametric four-wave-mixing field and a coupling of these fields with the driving laser field. A sharp onset of saturation of the parametric four-wave-mixing signals with sodium number density and a transition from a quadratic to a linear power dependence is observed. Both effects are explained in terms of the two-photon cancellation effect.
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.
If an extended Na vapor column (heat pipe configuration) is subjected to strong laser pumping near two-photon resonance with 3D3/2,5/2 or 4D3/2,5/2 states at pressures above tens of millitorr, strong stimulated emissions are produced by amplified spontaneous emission (ASE) or stimulated electron in hyper-Raman scattering (SEHRS) and by phase matched parametric four-wave mixing (PFWM). These new electromagnetic fields that are generated within the near-resonant nonlinear medium can strongly influence the total atomic response and produce several saturation and total cancellation types of effect.
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.