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Physical Review A

Two-photon resonant multiphoton ionization and stimulated emission in krypton and xenon

John C. Miller

Published Dec 1, 1989• 70 citations
Publisher

Abstract

Forward- and backward-directed, stimulated emissions have been observed following two-photon pumping of the 5p states of krypton and the 6p', 7p, 8p, and 4f states of xenon. Multiphoton ionization spectra are also obtained and compared with the photon-detected excitation spectra. In krypton coherent emissions from the 5p states to the 5s are observed, and for xenon many p\ensuremath{\rightarrow}s, d\ensuremath{\rightarrow}p, and f\ensuremath{\rightarrow}d cascade emissions are observed. By analogy to the well-studied alkali-metal and alkaline-earth examples, the emissions are assigned as amplified spontaneous emission. Several intensity anomalies in the xenon p\ensuremath{\rightarrow}s emissions are not understood at present. Interference effects due to coherent cancellation between competing excitation pathways may be occurring.

DOI
10.1103/physreva.40.6969

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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.

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Annual Meeting Optical Society of America•Jan 1, 1987•0 citations
Forward- and backward-directed, stimulated emissions have been observed following two-photon pumping of the 5p states of krypton and the 6p', 7p, 8p, and 4f states of xenon. Multiphoton ionization spectra are also obtained and compared with the photon-detected excitation spectra. In krypton coherent emissions from the 5p states to the 5s are observed, and for xenon many p\ensuremath{\rightarrow}s, d\ensuremath{\rightarrow}p, and f\ensuremath{\rightarrow}d cascade emissions are observed. By analogy to the well-studied alkali-metal and alkaline-earth examples, the emissions are assigned as amplified spontaneous emission. Several intensity anomalies in the xenon p\ensuremath{\rightarrow}s emissions are not understood at present. Interference effects due to coherent cancellation between competing excitation pathways may be occurring.
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.
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.
Multiphoton ionization (MPI) and third-harmonic generation (THG) in xenon and krypton have been studied via three-photon resonance with the xenon 6s'[1/2]10{[1/2]}_{1}^{0}[1/2]10​ and krypton 5s[(3/2]10{[(3/2]}_{1}^{0}[(3/2]10​ states. A second, tunable dye laser is used to couple these states to higher-lying even-parity states. Observations are reported regarding the third-harmonic related cancellation of the intermediate s-state population and the mechanisms of population of the final states. Effects of the four-photon resonance on THG are detailed. Changes induced by the second laser reduce THG in normally favorable regions and enable it in otherwise forbidden regions. Striking effects in the MPI spectra due to the changes induced in THG are reported.
Stimulated emission (SE) induced by pulsed two-photon excitation of the 6p′[1/2]0, 6p′[3/2]2, 7p[1/2]0, 7p[3/2]2, and 7p[5/2]2 states of the Xe atom has been studied. Spectra of SE were recorded in the 800–3500 nm region, which covers the 6p′, 7p → 7s (2500–3500 nm), 6p′, 7p → 5d (1000–2000 nm), 7s → 6p (1200–1900 nm) transitions, as well as the near-IR 6p → 6s (800–1000 nm) transitions. It is shown that excitation of the 7p states results in radiative cascade via the 7s states, 7p → 7s → 6p, although at least one case of cascading via the 5d states is also observed. Spectra of SE induced by excitation of the 6p′ states are dominated by the 6p′ → 6s′ transitions in the near IR and the 6p′ → 5d[1/2]1 → 6p[1/2]1 → 6s[3/2]1 cascade; the 6p′ → 7s → 6p cascade is also observed, although the secondary 7s → 6p emission is rather weak in comparison with excitation of the 7p states.
Resonantly enhanced multiphoton ionization signals through the 6s[32]J=16s[\frac{3}{2}]J=16s[23​]J=1 state of Xe rapidly disappear at pressures above 0.30 Torr; concurrently, intense, vacuum-ultra-violet third-harmonic radiation is detected in the forward direction. Laser excitation spectra of the vacuum ultraviolet light exhibit increasing blue shifts and bandwidths with increasing pressure. The observed competition between ionization and third-harmonic generation is discussed in terms of a model involving fast collective emission.
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.