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Journal of Physics B Atomic Molecular and Optical Physics

Parametric four-wave mixing in Kr

Koichi Tsukiyama∥

Published Apr 28, 1996• 12 citations
Publisher

Abstract

Parametric four-wave mixing in Kr is described. When the 5p levels of Kr were excited by two-photon absorption of pulsed UV laser radiation, near-infrared radiation corresponding to , as well as a resonance line at 123.6 nm, were observed. It was demonstrated that both near-infrared and vacuum ultraviolet emission were highly directional. Polarization properties of near-infrared radiation are presented.

DOI
10.1088/0953-4075/29/8/006

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Parametric four-wave mixing in Kr is described. When the 5p levels of Kr were excited by two-photon absorption of pulsed UV laser radiation, near-infrared radiation corresponding to , as well as a resonance line at 123.6 nm, were observed. It was demonstrated that both near-infrared and vacuum ultraviolet emission were highly directional. Polarization properties of near-infrared radiation are presented.
Two-photon resonant optical processes, using potassium ns2S1/2 states (7 ≤ n ≤ 20), are investigated in detail by a pulsed dye laser. About 100 coherent lines between 288–422 nm are generated through the processes ωUV ± ωIR = 2ωL and [Formula: see text]. The strongest lines (near mP–4S transitions) are formed by parametric oscillation and are generally split into components that are frequency shifted relative to atomic transitions. About 70 lines are generated by six-wave mixing processes and 15 other lines by four-wave mixing processes. The wavelengths, relative intensities of the lines, and the components of the strongest lines are explained with a theoretical analysis based on the wave equation, atomic polarization, and phase-match condition for both wave-mixing processes and parametric oscillations.
Two-photon resonant and near-resonant four-wave difference-frequency mixing in gases in the interaction regime when laser pulse durations are comparable to or shorter than the medium polarization relaxation time ${T}_{2}^{\ensuremath{'}}$ is investigated. The results of experimental studies of the process in Ar and Kr using pump pulses from the ArF-excimer laser are presented demonstrating a generation of tunable short pulse radiation in the range 102--124 nm. The results are discussed in terms of a theoretical model based on a self-consistent solution of the Bloch equations for the atomic transitions and the Maxwell equations for the fields. This enables one to interpret specific nonstationary resonant and quasiresonant phenomena involved in the frequency conversion process. It is shown that the femtosecond-pulse four-wave frequency-mixing technique with probe pulses significantly shorter than the pump pulses makes it possible to study the coherent dynamics of an atomic transition exposed to an intense field. Using atomic Kr as the nonlinear medium, coherent Rabi oscillations and the subsequent phase relaxation of excitation were observed under the condition of two-photon interaction of Kr with femtosecond 193-nm laser pulses. The obtained information is important for controlling and optimizing processes of two-photon resonant frequency conversion and for time-resolved studies of Rydberg states in atoms and molecules.
The nonlinear interaction of neutral krypton atoms with picosecond 193-nm radiation with intensities ≤1013 W/cm2 has been studied. Because of the relatively high intensity of the applied radiation field and the two-photon resonance of the 4p–6p transition, several competing nonlinear processes were observed that result in the generation of coherent radiation. Amplified spontaneous emission (ASE) from the two-photon-resonant level was observed in the IR frequency at ~2 μm. Additionally, a tunable IR wave, in the same frequency range, was generated by stimulated hyper-Raman scattering of the incident laser. The observed self-generated IR waves induced other nonlinear interactions, which resulted in the generation of extreme-ultraviolet (XUV) radiation in the same medium. Tunable XUV frequency was shown to be generated by four-wave sum mixing of the laser and the hyper-Raman wave. Vacuum-ultraviolet frequency was shown to be generated by four-wave oscillation, and other nontunable XUV frequencies resulted from anti-Stokes Raman scattering of the ASE IR waves.
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.
Optically inverted barium ions in the 6p(12)6{p}_{(\frac{1}{2})}6p(21​)​ excited state served as the nonlinear medium for doubly resonant four-wave parametric generation of coherent radiation at 167 nm. The excited barium ions were produced via selective autoionization. Stimulated-emission photons at 650 nm corresponding to the $6{p}_{(\frac{1}{2})}\ensuremath{-}5{d}_{(\frac{3}{2})}$ transition were mixed with input 451-nm laser photons turned to the $6{p}_{(\frac{1}{2})}\ensuremath{-}6{f}_{(\frac{5}{2})}$ two-photon resonance to produce the 167-nm output photons.