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Photonics

Monochromatic Conical IR Emission from Decaying KrF Laser Filaments in Xenon as Coherent Stimulated Four-Wave Mixing Process

Igor V. Smetanin, Alexey V. Shutov, N. N. Ustinovskii, Vladimir D. Zvorykin, Anna V. Bogatskaya, A. M. Popov

Published Feb 12, 2021• 0 citations
Publisher

Abstract

We develop theoretical background for the new nonlinear optical phenomenon of narrowly directed monochromatic IR conical emission which has been recently observed when 248-nm UV filaments propagate in xenon (V. D. Zvorykin, et al., Laser Phys. Lett. 13, 125404 (2016)). We treat it as coherent stimulated four-wave mixing process in which two pump KrF laser photons are converted into the coupled pair of resonance IR(828 nm) and VUV (147 nm) photons through 5p5(2P3/2)6p[1/2]0→5p5(2P3/2)6s[3/2]1o and 5p5(2P3/2)6s[3/2]1o→1S0 transitions. We explore the coherent interaction regime which proceeds at a time scale shorter than transverse relaxation time T2. The momentum and energy conservation laws determine the characteristic angle of conical emission. We find that the threshold of this coherent process is determined by the KrF laser pump pulse area.

DOI
10.3390/photonics8020047

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We develop theoretical background for the new nonlinear optical phenomenon of narrowly directed monochromatic IR conical emission which has been recently observed when 248-nm UV filaments propagate in xenon (V. D. Zvorykin, et al., Laser Phys. Lett. 13, 125404 (2016)). We treat it as coherent stimulated four-wave mixing process in which two pump KrF laser photons are converted into the coupled pair of resonance IR(828 nm) and VUV (147 nm) photons through 5p5(2P3/2)6p[1/2]0→5p5(2P3/2)6s[3/2]1o and 5p5(2P3/2)6s[3/2]1o→1S0 transitions. We explore the coherent interaction regime which proceeds at a time scale shorter than transverse relaxation time T2. The momentum and energy conservation laws determine the characteristic angle of conical emission. We find that the threshold of this coherent process is determined by the KrF laser pump pulse area.
Excitation of xenon near the two-photon resonance between the ground state and the 6p(1/2,0) state produces forward conical emission at a wavelength close to the 828-nm 6p(1/2,0)—6s(3/ 2,1) excited-state transition. We describe experimental features of this process as excited by 600-ps pulses of 250-nm radiation from a frequency-doubled dye laser with intensity up to 1.3 × 108 W/ cm2 in xenon at pressures of 1-20 Torr. The conical emission occurs most prominently when the driving field is a few gigahertz above the frequency at which spontaneous emission from the excited 6p state peaks. The cone angle increases with xenon pressure in the 1-10-Torr range. The dependence appears consistent with the predictions based on noncollinearly phase-matched four-wave mixing. In this interpretation, the fourth wave would be near resonance with the 146.9-nm first resonance transition of xenon and detuned to the low-frequency side. The conical emission co-exists (and may compete with) an axial stimulated process which may be either two-photon driven amplified spontaneous emission or stimulated hyper-Raman scattering. The different tuning characteristics for the two processes make the extent of their competition unclear.
Both on-axis and conical emissions have been observed following two-photon pumping of the 5p states of krypton and the 6p', 7p, 8p, and 4f states of xenon. In the former case, coherent emissions from the 5p states to the 5s are observed, and in the latter case, many p..-->..s, d..-->..p, and f..-->..d cascade emissions are observed. By analogy to the well-studied alkali and alkaline earth examples, the emissions are discussed in terms of amplified spontaneous emission (ASE), stimulated hyper-Raman scattering, and parametric four-wave mixing. The physical processes responsible for the conical emission and for intensity anomalies in the xenon p..-->..s emissions are not understood at present. Interference effects due to coherent cancellation between competing excitation pathways may be occurring. 4 refs., 3 figs.
Both on‐axis and conical emissions have been observed following two‐photon pumping of the 5p states of krypton and the 6p’, 7p, 8p, and 4f states of xenon. In the former case, coherent emissions from the 5p states to the 5s are observed and in the latter case, many p → s, d → p, and f → d cascade emissions are observed. By analogy to the well‐studied alkali and alkaline earth examples, the emissions are discussed in terms of amplified spontaneous emission (ASE), stimulated hyper‐Raman scattering, and parametric four‐wave mixing. The physical processes responsible for the conical emission and for intensity anomalies in the xenon p → s emissions are not understood at present. Interference effects due to coherent cancellation between competing excitation pathways may be occurring.
A pulsed dye-laser beam (ωL) pumped by a frequency-doubled Nd:YAG laser is focused into a heat-pipe oven containing potassium vapor (nk ≈ 1016 cm−3). Two-photon resonant four-wave and six-wave mixing processes using the potassium 8s 2S1/2 state are investigated. Thirty-two coherent UV radiation lines are generated within the range of 300–400 nm through the processes ωUV = 2ωL ± ωIR and ωUV = 2ωL − ω′IR − ω″IR ± ω‴IR, where ωIR are frequencies of laser-induced IR waves generated in the vapor near the transitions 8S–7P, 7P–7S, 7P–5D, 8S–6P, 7S–6P, 5D–6P, etc. The influence of resonant enhancement on the UV line intensities and the phase-matching condition are analyzed.
The interaction of a laser with potassium atoms is investigated by monitoring the radiation of the 5P-4S transition under the two-photon 4S(1/2)-6S(1/2) excitation. For low number density and laser intensity the observed radiation is parametric axial or conical, depending on the laser detuning from the two-photon resonance, the number density and the laser intensity. With increasing laser intensities and number densities, an additional delayed component is observed corresponding to a two-step four-wave mixing with the participation of internally generated photons. A two-photon quantum interference effect is observed for the total (axial and conical) parametric four-wave mixing emission. A deviation from the proposed model under certain experimental parameters is attributed to a two-step four-wave mixing and the phase mismatch of the parametric processes.