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Journal of Applied Physics

Excitation of highly excited states by collisions between two excited cesium atoms

Scott G. Leslie, J. T. Verdeyen, W. Millar

Published Nov 1, 1977• 27 citations
Publisher

Abstract

Fluorescence from highly excited atomic states has been observed in cesium vapor irradiated by a dye laser tuned to either one of the 62S–72P transitions. The emission originated from levels as high as 1 eV above the state being pumped. The high-lying states are believed to be excited by an electronic energy transfer induced in a collision of two atoms occupying lower excited levels.

DOI
10.1063/1.323473

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Canadian Journal of Physics•Sep 1, 1974•8 citations
Fluorescence from highly excited atomic states has been observed in cesium vapor irradiated by a dye laser tuned to either one of the 62S–72P transitions. The emission originated from levels as high as 1 eV above the state being pumped. The high-lying states are believed to be excited by an electronic energy transfer induced in a collision of two atoms occupying lower excited levels.
The method of sensitized fluorescence has been employed to investigate the [Formula: see text] excitation transfer processes in cesium induced in collisions with ground state cesium atoms. The cesium vapor density was kept sufficiently low to enable the cross sections for the mixing process to be determined under single collision conditions and to ensure that radiation trapping and quenching were negligible. A nitrogen laser pumped dye laser was used to excite the cesium atoms to each of the 72P levels in turn and measurements of the relative intensities of fluorescence yielded the following cross sections: [Formula: see text] These results are consistent with the empirical relationship between the magnitude of the cross sections and the fine structure splitting that has previously been determined for the alkalis.
We report an application of laser spectroscopy techniques to a study of collision-induced interactions in atomic excited states. Due to pulsed dye laser excitation a considerable selective population of highly excited states of ccsium is obtained. Collision-induced transfer of excitation energy between the excited states results in modifications in time and spectral characteristics of observed atomic fluorescence. Quantitative information on the efficiency of collisional processes can be obtained from the measurements of time constants of the time-resolved fluorescence signals and/or from those of the integrated intensities of the fluorescence lines. Both possibilities are used in the present work. Perturbation of nD (n=8-14) and nS (n=1O-15) states of cesium in collisions with noble-gas atoms is investigated. The cross sections for the transfer of excitation between fine-structure substates of the nD states (J mixing) and for the nS-(n-4)F intermultiplet transfer are obtained.
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 fluorescence spectrum of cesium vapor was studied in a cell irradiated with the light of 852.3 nm resonance line from a single mode laser diode. From the intensities and spectra of the Cs and Cs2 fluorescence we identified several collisional and radiative processes in the excited cesium atom-dimer system. The atomic lines of the highly excited states were the result of collisional energy transfer from Cs(6P 3/2) + Cs(6P 3/2) to Cs(6D, 8S) atoms. The Cs2 (B 1 IIu) band formed in Cs (6P) + Cs2 (X1sigmag+) collisions. The fine-structure mixing in 6 2P atoms was studied through excitation transfer, energy-pooling collision, and collisional excitation transfer between Cs2 and Cs. The authors estimated the value of rate coefficient for the collisional energy transfer from 6P3/2 to 6P1/2 to be (5.2+/-2.1) x 10(-11) cm3 x s(-1). For the excitation transfer process Cs2 (B 1 IIu)+ Cs(6S)--> Cs2 (X 1sigmag+) + Cs(6P1/2 ), a rate coefficient of (1.0+/-0.4) x 10(-9) cm3 x s(-1) was yielded.
The cross sections for excitation transfer between the 62P fine structure levels of rubidium, induced in collisions with ground state rubidium atoms, have been measured using a nitrogen laser pumped dye laser as the optical excitation source in a fluorescence experiment. Rubidium vapor was irradiated with each component of the 2P rubidium doublet in turn, and measurements of the relative intensities of fluorescence yielded the following cross sections: [Formula: see text] These results are consistent with the empirical relationship between the magnitude of the cross sections and the fine structure splitting that has previously been established for the alkalis.