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Chinese Journal of Chemical Physics

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, Xueyang Li, Jingwei Guo, Jinbo Liu, Shu Hu, Hui Li, Peng‐Yuan Wang, Ying Chen, Fengting Sang, Yuqi Jin

Published Dec 1, 2018• 0 citations
Publisher

Abstract

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.

DOI
10.1063/1674-0068/31/cjcp1806142

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Journal of Baoji University of Arts and Sciences•Jan 1, 2009•0 citations
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.
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.
Using stepwise excitation of the cesium 8S atoms level in Cs vapor,several collisional and radiative processes have been identified from the intensities and spectra of the Cs fluorescence.The 5D state was populated by 8S→7P→5D transitions.In cesium densities 1016-1017?cm-3,the energy pooling collisions 5D+5D→nL+6S(nL=9D,11S,7F are studied.Since the 5D→6P(3.0-3.6 μm) fluorescence could not be detected with this experiment,the EP rate coefficients have been measured relative to the known rate coefficient of the collision,i.e.,6P+5D→6S+7D.The excited-atom density and spatial distribution were mapped by monitoring the absorption of a counterpropagating single-mode laser beam,tuned to 6P3/2→8S1/2 transition,which could be translated parallel to the pump beam.The excited atom densities are combined with measured fluorescene ratios to determine cross sections for the cesium energy pooling process.The average values(in units of 10-10?cm3s-1) for nL=9D,11S and 7F are 8.4±4.2,7.3±3.6,and 9.7±4.8,respectively.Influence on k11S and k7F of the energy transfer process 11S+6S7F+6S is also dicussed.
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.
We report experimentally the measured rate coefficients for the energy pooling (EP) collisions process Cs(5D)+Cs(5D)-gCs(6S)+Cs(nL=9D,11S,7F) in cesium densities of 10^(16)-10^(17) cm^(-3). The 5D state was populated via 8S-g7P-g5D spontaneous emission following two-step pumping 6S-g6P_(3/2)-g8S. Since the 5D-g6P (3.0-3.6 microns) fluorescence could not be detected in this experiment, we carried out a relative measurement for the process 6P+5D-g6S+7D. The excited-atom density and spatial distribution were mapped by monitoring the absorption of a counterpropagating single-mode laser beam, tuned to 6P_(3/2)-g9S_(1/2) transition, which could be translated parallelly to the pump beam. The excited atom densities have been combined with the measured fluorescence ratios to yield EP rate coefficients. The average values for nL=9D,11S and 7F are 8.0+-4.0, 7.0+-3.5, and 9.3+-4.6 (in units of 10^(-10) cm3/s), respectively. Influence of the energy transfer process 11S+6S-g7F+6S on the rate coefficients k_(11S) and k_(7F) is also discussed.
Energy-transfer collisions between two 6 2^{2}2S1/2{\mathit{S}}_{1/2}S1/2​ laser-excited indium atoms leading either to ionization of one of the colliding atoms or to population of its n2{\mathit{n}}^{2}n2P Rydberg states, have been studied. Atomic lines corresponding to the 5s5p2{\mathit{p}}^{2}p2 2^{2}2D\ensuremath{\rightarrow}5${\mathit{s}}^{2}$6p 2^{2}2P1/2,3/2{\mathit{P}}_{1/2,3/2}P1/2,3/2​ interconfiguration transitions have been recorded as evidence of the energy-pooling ionization via an autoionizing state. Atomic lines corresponding to the n2{\mathit{n}}^{2}n2P\ensuremath{\rightarrow}6 2^{2}2S transitions for n=9, 10, and 11 as well as to the 5 2^{2}2D\ensuremath{\rightarrow}5 2^{2}2P transitions have proven that the population of highly excited indium atomic states is through the energy-poolimg collisions.
Aim An experimental study into cesium energy pooling collision,Cs(6P3/2)+Cs(6P3/2)→Cs(nLJ=8S1/2,4F5/2,4F7/2)+Cs(6S1/2),has been carried out in a cell.Methods A single mode semiconductor laser is used to excite the 6P3/2 state,the other single mode laser antiparallel to pumping laser is used as absorption line to detect excited atomic intensity and its spatial distribution,with absorption line transiting from 6P3/2 to 8S1/2 and parallel to the movement of pumping laser.The cross section of energy pooling collisions is obtained by the ratio of the excited atomic density to fluorescence intensity of the spectral line.Results The cross sections of 8S1/2,4F5/2 and 4F7/2 are(5.43±1.56)×10-16 cm2,(4.89±1.16)×10-16 cm2 and(6.17±1.60)×10-16 cm2,respectively.Conclusion Compared with other test results,the calculation results are exact.