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The Journal of Chemical Physics

Stimulated directional emission induced by two-photon excitation of the Xe 6p′ and Xe 7p states

Vadim A. Alekseev, Peter J. M. van der Burgt, Donald W. Setser

Published Mar 3, 2017• 1 citation
Publisher

Abstract

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.

DOI
10.1063/1.4977522

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A pulsed source for Xe(6s[3/2]1) and Xe(6s′[1/2]1) resonance state atoms using two-photon driven amplified spontaneous emission from the Xe(6p) and Xe(6p′) states

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A new, simple method for the generation of Xe(6s[3/2]1) and Xe(6s′[1/2]1) atoms is described. The method involves resonant two-photon excitation of Xe(6p[1/2]0 and 6p′[3/2]2) states followed by amplified spontaneous emission (ASE) to the Xe(6s[3/2]1 and 6s′[1/2]1) states. The vacuum ultraviolet transitions, Xe(6s[3/2]1→5p6(1S0)) at 147 nm and Xe(6s′[1/2]1→5p6(1S0)) at 129.6 nm, were used to monitor the time dependence of the resonance state atom concentrations. The quenching rate constants of these resonance atoms with ten molecules were measured at 300 K. The quenching cross-sections of the Xe(6s and 6s′) resonance atoms are compared to the cross-sections of the metastable Xe(6s[3/2]2) atoms and Xe(6p[3/2]2) atoms. The correlation between quenching cross-sections and photoabsorption cross-section of the molecules predicted by the resonance dipole–dipole energy transfer model is discussed. The applicability of the two-photon driven ASE method for the generation of other resonance state atoms is considered.

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

John C. Miller

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.

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Conical emission in atomic xenon

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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.

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Energy-Transfer Kinetics for Xe (6p[1/2]0) Atoms in Kr, Ar, Ne, and He

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The kinetic processes for the Xe (6p[1/2] 0 ) atoms in Kr, Ar, Ne, and He buffer gases were studied. We found that Kr, Ar, and Ne atoms can be used to switch the amplified spontaneous emission (ASE) channel from 3408 nm (6p[1/2] 0 –6s′[1/2] 1 ) to 3680 nm (5d[1/2] 1 –6p[1/2] 1 ), while Xe and He atoms do not show such a phenomenon. This ASE channel switch is mainly ascribed to the fast transfer of 6p[1/2] 0 → 5d[1/2] 1 . On the basis of the rate equations for two-state coupling (energy-transfer processes between the two states are very rapid), the reason why the ASE channel switch effect normally coincides with a double exponential decay of the spontaneous emission at 828 nm (6p[1/2] 0 –6s[3/2] 1 ) is explained. The actual situations in Xe, Ar, Ne, and He follow this rule. However, the strictly single exponential decay of the spontaneous emission at 828 nm and strong ASE channel switch effect simultaneously emerge in Kr. This indicates that the transfer of 6p[1/2] 0 → 5d[1/2] 1 in Kr does not occur via two-state coupling, but via two steps of near-resonance collision through the 5s[3/2] 2 (Kr) state as the intermediate state (6p[1/2] 0 → 5s[3/2] 2 (Kr) → 5d[1/2] 1 ). In addition, we found Xe (6p[1/2] 0 ) atoms strongly tend to reach the 6p[3/2] 2, 6p[3/2] 1, and 6p[5/2] 2 states through the 5s[3/2] 2 (Kr) state as the intermediate state in Kr. The 5s[3/2] 2 (Kr) state plays a very important role in the energy-transfer kinetics for the Xe (6p[1/2] 0 ) atoms. Kr is probably an excellent buffer gas for laser systems based on Xe.

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Energy-transfer processes of Xe (6p[1/2], 6p[3/2]2, and 6p[5/2]2) atoms under the condition of ultrahigh pumped power

Shan He, Junzhi Chu, Dong Liu +9 more

The kinetic processes of Xe (6p[1/2]0, 6p[3/2]2, and 6p[5/2]2) atoms under the focused condition were investigated. The atomic density of the laser prepared state significantly increases. Therefore, the probability of the energy-pooling between two high-lying atoms increases. There are three major types of the energy-pooling collisions. The first type is the energy-pooling ionization. Once the excitation laser is focused, the obvious ionization can be observed from the side window whenever the laser prepared state is 6p[1/2]0, 6p[3/2]2, or 6p[5/2]2 state. Ionization of Xe is attributed to the energy-pooling ionization or a Xe* atom reabsorbing another excitation photon. The second type is energy-pooling with big energy difference. When the 6p[1/2]0 state is the laser prepared state, the energy-pooling collision between two 6p[1/2]0 atoms can produce one 5d[3/2]1 atom and one 6s′[1/2]0 atom. The third type is energy-pooling with small energy difference. The intensities of fluorescence lines are much stronger that five secondary 6p states act as the upper states, and the rising edges of these fluorescence lines are much steeper. The primary mechanism of generating the secondary 6p atoms is energy-pooling collision instead of collision relaxation. Based on the collision probability, the rate of energy-pooling between two 6p[1/2]0 atoms is deduced (6.39 × 108 s−1). In addition, the 6s atoms also increase under the focused condition. Therefore, all the fluorescence lines are serious trailing by radiation trapping.

Chinese Journal of Chemical Physics•Dec 1, 2018•0 citations

Two-photon resonant, stimulated processes in krypton and xenon

Joel C. Miller

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
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.
A new, simple method for the generation of Xe(6s[3/2]1) and Xe(6s′[1/2]1) atoms is described. The method involves resonant two-photon excitation of Xe(6p[1/2]0 and 6p′[3/2]2) states followed by amplified spontaneous emission (ASE) to the Xe(6s[3/2]1 and 6s′[1/2]1) states. The vacuum ultraviolet transitions, Xe(6s[3/2]1→5p6(1S0)) at 147 nm and Xe(6s′[1/2]1→5p6(1S0)) at 129.6 nm, were used to monitor the time dependence of the resonance state atom concentrations. The quenching rate constants of these resonance atoms with ten molecules were measured at 300 K. The quenching cross-sections of the Xe(6s and 6s′) resonance atoms are compared to the cross-sections of the metastable Xe(6s[3/2]2) atoms and Xe(6p[3/2]2) atoms. The correlation between quenching cross-sections and photoabsorption cross-section of the molecules predicted by the resonance dipole–dipole energy transfer model is discussed. The applicability of the two-photon driven ASE method for the generation of other resonance state atoms is considered.
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.
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.
The kinetic processes for the Xe (6p[1/2] 0 ) atoms in Kr, Ar, Ne, and He buffer gases were studied. We found that Kr, Ar, and Ne atoms can be used to switch the amplified spontaneous emission (ASE) channel from 3408 nm (6p[1/2] 0 –6s′[1/2] 1 ) to 3680 nm (5d[1/2] 1 –6p[1/2] 1 ), while Xe and He atoms do not show such a phenomenon. This ASE channel switch is mainly ascribed to the fast transfer of 6p[1/2] 0 → 5d[1/2] 1 . On the basis of the rate equations for two-state coupling (energy-transfer processes between the two states are very rapid), the reason why the ASE channel switch effect normally coincides with a double exponential decay of the spontaneous emission at 828 nm (6p[1/2] 0 –6s[3/2] 1 ) is explained. The actual situations in Xe, Ar, Ne, and He follow this rule. However, the strictly single exponential decay of the spontaneous emission at 828 nm and strong ASE channel switch effect simultaneously emerge in Kr. This indicates that the transfer of 6p[1/2] 0 → 5d[1/2] 1 in Kr does not occur via two-state coupling, but via two steps of near-resonance collision through the 5s[3/2] 2 (Kr) state as the intermediate state (6p[1/2] 0 → 5s[3/2] 2 (Kr) → 5d[1/2] 1 ). In addition, we found Xe (6p[1/2] 0 ) atoms strongly tend to reach the 6p[3/2] 2, 6p[3/2] 1, and 6p[5/2] 2 states through the 5s[3/2] 2 (Kr) state as the intermediate state in Kr. The 5s[3/2] 2 (Kr) state plays a very important role in the energy-transfer kinetics for the Xe (6p[1/2] 0 ) atoms. Kr is probably an excellent buffer gas for laser systems based on Xe.
The kinetic processes of Xe (6p[1/2]0, 6p[3/2]2, and 6p[5/2]2) atoms under the focused condition were investigated. The atomic density of the laser prepared state significantly increases. Therefore, the probability of the energy-pooling between two high-lying atoms increases. There are three major types of the energy-pooling collisions. The first type is the energy-pooling ionization. Once the excitation laser is focused, the obvious ionization can be observed from the side window whenever the laser prepared state is 6p[1/2]0, 6p[3/2]2, or 6p[5/2]2 state. Ionization of Xe is attributed to the energy-pooling ionization or a Xe* atom reabsorbing another excitation photon. The second type is energy-pooling with big energy difference. When the 6p[1/2]0 state is the laser prepared state, the energy-pooling collision between two 6p[1/2]0 atoms can produce one 5d[3/2]1 atom and one 6s′[1/2]0 atom. The third type is energy-pooling with small energy difference. The intensities of fluorescence lines are much stronger that five secondary 6p states act as the upper states, and the rising edges of these fluorescence lines are much steeper. The primary mechanism of generating the secondary 6p atoms is energy-pooling collision instead of collision relaxation. Based on the collision probability, the rate of energy-pooling between two 6p[1/2]0 atoms is deduced (6.39 × 108 s−1). In addition, the 6s atoms also increase under the focused condition. Therefore, all the fluorescence lines are serious trailing by radiation trapping.
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.