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The Journal of Physical Chemistry A

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

Shan He, Dong Liu, Xueyang Li, Junzhi Chu, Jingwei Guo, Jinbo Liu, Shu Hu, Fengting Sang, Yuqi Jin

Published May 29, 2018• 6 citations
Publisher

Abstract

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.

DOI
10.1021/acs.jpca.8b03238

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Stark shift/broadening by stimulated emission

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Collisional relaxation in 5(2)P potassium atoms.

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Collisional excitation transfer and relaxation of K 5$\\sp2$P atoms in collisions with noble gases, as well as the radiative lifetimes of the K 5P, 6P and 7P fine-structure states have been investigated by methods of atomic fluorescence spectroscopy. Potassium vapour was mixed in a cell with a noble gas and selectively excited by pulsed dye-laser radiation to the 5$\\sp2$P$\\sb{1\\over2}$ or the 5$\\sp2$P$\\sb{3\\over 2}$ state in zero magnetic field and to the 5$\\sp2$P$\\sb{{1\\over 2}-{1\\over 2}}$ or the 5$\\sp2$P$\\sb{{3\\over 2}-{3\\over 2}}$ Zeeman substate in a field of 70 kG. Interferometric analysis of the fluorescence emitted from the directly (optically) excited state and that emitted from the collisionally populated states allowed the determination of the fine-structure mixing cross sections for collisions with He, Ne, Ar, Kr and Xe in zero magnetic field. Excitation transfer between Zeeman substates was investigated for collisions between the selectively excited 5P atoms and He, Ne and Ar atoms, allowing the determination of the multipole relaxation (depolarization) cross sections for dipole, quadrupole and octupole decay, as well as the Zeeman and fine-structure mixing cross sections and orientation transfer cross sections. A comparison of theoretical calculations with the experimental data has been made and the rate equations governing multipole relaxation and including effects due to strong fine-structure mixing on the multipole relaxation, have been described in detail. The radiative lifetimes of the individual fine-structure components of the K 5P, 6P and 7P states have been determined experimentally by means of time-resolved laser-induced fluorescence techniques. These data are compared with numerous theoretical calculations and the available experimental values.Dept. of Physics. Paper copy at Leddy Library: Theses & Major Papers - Basement, West Bldg. / Call Number: Thesis1988 .B474. Source: Dissertation Abstracts International, Volume: 49-04, Section: B, page: 1223. Thesis (Ph.D.)--University of Windsor (Canada), 1988.

•Jan 1, 1988•0 citations
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.
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.
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.
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.
The kinetic behaviors of 6p[1/2]0, 6p[3/2]2 ,and 6p[5/2]2 were examined under the ultrahigh pumped power. These processes were detected by the way of time-resolved fluorescence and ASE spectra. A theory of energy-pooling is presented under the focused condition. There are three types of energy-pooling processes. The first type is energy-pooling ionization. The obvious ionization can be observed whenever the laser prepared state is the 6p[1/2]0, 6p[3/2]2, or 6p[5/2]2 state. The second type is energy-pooling with big energy difference. The energy-pooling collision between the two 6p[1/2]0 atoms can produce one 5d[3/2]1 atom and one 6s’[1/2]0 atom when the prepared state is 6p[1/2]0. The third type is energy-pooling with small energy difference. The way of generation of five secondary 6p states is energy-pooling instead of collision relaxation.
Previous experimental work by our group1 has shown that the two-photon excitation of the 6p[1/2,0] state of xenon has a fairly sharp threshold for the onset of amplified spontaneous emission (ASE) from the 6p[1/2,0] state to the excited 6s state. The excitation probability has the expected quadratic dependence on excitation intensity below the ASE threshold but an unexpected linear dependence above threshold. We hypothesize that the reduced excitation probability results from an ac Stark shift/broadening of 6p[1/2,0] state by the ASE field. We have numerically solved the coupled Maxwell-Bloch equations with and without the relevant Stark terms. The ASE threshold predicted by the numerical solutions occurs at an intensity about an order of magnitude higher than the experimental value. Because of uncertainties in some of the experimental parameters this difference is not unreasonable. Solution of the equations without Stark terms gives quadratic excitation dependence above the ASE threshold. Including the Stark terms reduces the dependence to a 1.2 power law. The change to a 1.2 power occurs ~50% above ASE threshold, whereas the experimental change occurs almost right at threshold.
Collisional excitation transfer and relaxation of K 5sp2\\sp2sp2P atoms in collisions with noble gases, as well as the radiative lifetimes of the K 5P, 6P and 7P fine-structure states have been investigated by methods of atomic fluorescence spectroscopy. Potassium vapour was mixed in a cell with a noble gas and selectively excited by pulsed dye-laser radiation to the 5sp2\\sp2sp2Psb1over2\\sb{1\\over2}sb1over2 or the 5sp2\\sp2sp2Psb3over2\\sb{3\\over 2}sb3over2 state in zero magnetic field and to the 5sp2\\sp2sp2Psb1over2−1over2\\sb{{1\\over 2}-{1\\over 2}}sb1over2−1over2 or the 5sp2\\sp2sp2Psb3over2−3over2\\sb{{3\\over 2}-{3\\over 2}}sb3over2−3over2 Zeeman substate in a field of 70 kG. Interferometric analysis of the fluorescence emitted from the directly (optically) excited state and that emitted from the collisionally populated states allowed the determination of the fine-structure mixing cross sections for collisions with He, Ne, Ar, Kr and Xe in zero magnetic field. Excitation transfer between Zeeman substates was investigated for collisions between the selectively excited 5P atoms and He, Ne and Ar atoms, allowing the determination of the multipole relaxation (depolarization) cross sections for dipole, quadrupole and octupole decay, as well as the Zeeman and fine-structure mixing cross sections and orientation transfer cross sections. A comparison of theoretical calculations with the experimental data has been made and the rate equations governing multipole relaxation and including effects due to strong fine-structure mixing on the multipole relaxation, have been described in detail. The radiative lifetimes of the individual fine-structure components of the K 5P, 6P and 7P states have been determined experimentally by means of time-resolved laser-induced fluorescence techniques. These data are compared with numerous theoretical calculations and the available experimental values.Dept. of Physics. Paper copy at Leddy Library: Theses & Major Papers - Basement, West Bldg. / Call Number: Thesis1988 .B474. Source: Dissertation Abstracts International, Volume: 49-04, Section: B, page: 1223. Thesis (Ph.D.)--University of Windsor (Canada), 1988.