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Annual Meeting Optical Society of America

Conical emission in atomic xenon

M. Rankin, Jon P. Davis, Christopher Giranda, M. Squicciarini, Lloyd C. Bobb

Published Jan 1, 1987• 0 citations
Publisher

Abstract

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.

DOI
10.1364/oam.1987.mi1

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Two-photon resonant, stimulated processes in krypton and xenon

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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.

•Nov 1, 1988•0 citations

Two-photon resonant, stimulated processes in krypton and xenon

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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.

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Annual Meeting Optical Society of America•Jan 1, 1986•0 citations

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Annual Meeting Optical Society of America•Jan 1, 1989•0 citations
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.
We describe collision studies on the two-photon excitation and fluorescence of the xenon 6p[1/2,0] excited state. Molecular nitrogen is the major collision partner. The 250-nm second harmonic of a line-narrowed Hansch-type dye laser excites the 6p state of xenon by two-photon absorption. Sample mixtures contain xenon at a partial pressure of 1 Torr and nitrogen at partial pressures of up to several hundred Torr. Time-resolved and time-integrated measurements of the intensity of the 828-nm 6p[1/2,0]—6s[3/2,1] allowed transition are obtained with photomultipliers, a transient digitizer, and a computerized data acquisition system. We extract pressure-dependent and pressure-independent components of the fluorescence lifetime and fluorescence yield from measurements over a range of nitrogen pressures. When the excitation power density is of the order of 104 W/cm2, the excited xenon atoms decay spontaneously. For spontaneous fluorescence, we obtain an inelastic (quenching) collision cross section of ~10–14 cm2 for xenon-nitrogen collisions, and a pressure-broadening coefficient of ~3 × 107 Hz/(Torr N2) for the two-photon transition rate. For excitation intensities above 2.6 × 106 W/cm2, the xenon atoms radiate cooperatively in a subnanosecond pulse. The fluorescence yield of this cooperative emission increases with nitrogen pressure rather than decreasing as in the spontaneous case. Mechanisms are discussed.
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.
Three-level systems in which the middle level has opposite parity from the remaining levels can develop optical gain on the excited-state transition when a two-photon resonant field couples the ground state with the uppermost state. Both population gain, which leads to amplified spontaneous emission, and hyper-Raman gain, which leads to stimulated hyper-Raman scattering, occur.1 Evidence for both types of process appears in two-photon-excited bidirectional emission in atomic xenon.2 This paper presents and compares threshold scaling characteristics, temporal behavior, directional energy distribution patterns, and tuning behavior as evidence for the gain mechanism in xenon. Near threshold, clear evidence for population inversion gain exists. Above threshold, axial emission energy exceeds off-axial (spontaneous emission) energy by a factor which increases with excitation energy. This excess of energy indicates the presence of hyper-Raman and/or four-wave mixing gain.