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Soviet Journal of Quantum Electronics

Four-wave parametric interaction of ultrashort optical pulses in a two-level system of barium atoms

David G. Sarkisyan, S O Sapondzhyan

Published Apr 30, 1984• 1 citation
Publisher

Abstract

An experimental investigation was made of a four-wave parametric interaction (FWPI) in a field of ultrashort optical pulses (λp ≈0.55 μ) acting on a 1S–1P0 two-level system of barium atomic vapor. It was observed that a pair of new frequencies ν3 and ν4 appeared as a result of FWPI, ν3 being close to ν'tps = 2νp – ν'sp and ν4 being close to ν'sp. This process was observed on approaching the resonance from the low-frequency side. When the resonance was approached from the high-frequency side, conical emission was recorded. It was found that a FWPI in a two-level system subjected to a strong pump field is governed by the third- and fifth-order nonlinear susceptibilities χ(3) and χ(5).

DOI
10.1070/qe1984v014n04abeh005045

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An experimental investigation was made of a four-wave parametric interaction (FWPI) in a field of ultrashort optical pulses (λp ≈0.55 μ) acting on a 1S–1P0 two-level system of barium atomic vapor. It was observed that a pair of new frequencies ν3 and ν4 appeared as a result of FWPI, ν3 being close to ν'tps = 2νp – ν'sp and ν4 being close to ν'sp. This process was observed on approaching the resonance from the low-frequency side. When the resonance was approached from the high-frequency side, conical emission was recorded. It was found that a FWPI in a two-level system subjected to a strong pump field is governed by the third- and fifth-order nonlinear susceptibilities χ(3) and χ(5).
A phosphate neodymium glass laser emitting picosecond pulses tunable in the 1.05–1.07 μ range was developed to study nonlinear optical processes in atomic barium vapor. Its temporal characteristics were investigated using a modified second harmonic beam method. Electron stimulated Raman scattering and four-photon parametric conversion in atomic barium vapor were used to obtain efficient conversion of the third harmonic of the picosecond phosphate laser (350–356 nm) to the Stokes (580–600 nm) and anti-Stokes (250–253 nm) waves. The highest conversion quantum efficiency for the Stokes wave was 15%. Electron stimulated Raman scattering in an (6 s 2 ) 1 S –(6 s 7 s ) 1 S –(6 s 6 p ) 1 P 0 system, having a strongly forbidden first transition, was recorded for the first time. In the same system, two-photon pumping generated four-photon parametric superradiance and it was found that the signal and idler waves had anomalously broad spectra (wider than 100 cm −1 ).
An investigation was made of a noncollinear transient four-wave parametric interaction in an atomic barium vapor subjected to the first and second harmonics of tunable neodymium-activated phosphate glass and YAG:Nd3+ lasers emitting picosecond pulses. Variation of the angle between the pump beams was used to control the characteristics of the signal and idler pulses. When the pump radiation was supplied only by a master oscillator, it was possible to generate relatively simply ultrashort pulses tunable near 0.98 μm. A comparison was made with a theory of transient four-wave parametric interaction, which was valid also in saturating pump fields.
Two-photon resonant or nearly resonant optical processes have been investigated in atomic barium vapour ( approximately 10 17 cm -3 ) with a pulse dye laser (frequency omega L ) covering the range 735-415 nm. These interactions result in strong coherent emissions emitted either forward and backward, or forward only. The optical processes responsible for these coherent emissions have been identified. Seventy five lines (frequency omega ES ) emitted from 1000 to 360 nm are due to optically pumped stimulated emissions or stimulated electronic hyper-Raman scattering. Twenty eight lines (frequency omega sigma ) observed from 795 to 250 nm are generated through four-wave-mixing parametric processes with omega sigma =2 omega L +or- omega ES , and nine- (795-260 nm) through six-wave-mixing parametric processes with omega sigma =2 omega L - omega ES1 - omega ES2 +or- omega ES3 .
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.
The problem of transient four-wave parametric interaction in a two-level medium is solved taking into account the group delay without assuming a weak exciting field. It is found that a high-power narrow peak whose duration τs is considerably shorter than the pump duration τp is observed against the background of a slowly varying envelope of the weak signal during its amplification process. In the case of a high pump intensity (ΩmτP−1) the lowest possible value of τS that can be achieved for a suitable angle of incidence and input signal frequency is governed by τp/Ωm1/2, where Ωm is the peak Stark shift of the resonance frequency.