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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Collision-induced energy transfer in intermediate excited states of cesium

M. Łukaszewski, I. Jackowska

Published Sep 24, 1993• 0 citations
Publisher

Abstract

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.

DOI
10.1117/12.155644

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•Sep 1, 2006•0 citations
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.
Cross sections for the transfer of excitation between fine-structure sublevels of the 9D state of caesium due to collisions with noble-gas atoms are measured. The experimental method employs stepwise excitation with a pulsed dye laser in the second step (6 2 P 3/2 to 9 2 D 5/2 ) and time-resolved detection of sensitised fluorescence 9 2 D 3/2 to 6 2 P 1/2 . The cross sections for the process Cs(9 2 D 3/2 )+A to Cs(9 2 D 5/2 )+A are (in units of 10 -14 cm 2 ) 7.6(1.5), 2.5(5), 2.7(5), 3.0(6) and 3.2(6) for A=He, Ne, Ar, Kr and Xe, respectively. For all the noble gases except helium the experimental cross sections are a few times smaller than the ones obtained in a recent semiclassical calculation.
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.
The 8 2S^{2}S2S state of rubidium is selectively populated by stepwise excitation using light from a rubidium lamp and a tunable dye laser. Excitation transfer from the 8 2S^{2}S2S to the 6 2D^{2}D2D state is studied in a glass cell containing rubidium vapor and noble-gas atoms at different pressures and ground-state rubidium atoms as perturbers. The thermally averaged cross sections for excitation transfer (in units of ${10}^{\mathrm{\ensuremath{-}}15}$ cm2{\mathrm{cm}}^{2}cm2) are 0.13\ifmmode\pm\else\textpm\fi{}0.05, 3.0\ifmmode\pm\else\textpm\fi{}1.2, 2.2\ifmmode\pm\else\textpm\fi{}0.9, 1.7\ifmmode\pm\else\textpm\fi{}0.7, and 4.3\ifmmode\pm\else\textpm\fi{}2.6 for the noble gases He, Ne, Ar, Kr, and Xe, respectively, and (6.7\ifmmode\pm\else\textpm\fi{}3.0)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}13}$ cm2{\mathrm{cm}}^{2}cm2 for rubidium atoms. The results show that the excitation-transfer cross sections for intermediately excited states cannot be accurately scaled from simple models.
Collisions of excited 113Cd(5 3P1) atoms with various molecular gases (N2, H2, D2, CO, CO2, CH4, C2H6, C2H4, O2) have been investigated using atomic fluorescence spectroscopy. By selective excitation of a hyperfine structure level with a pulsed dye laser and studying the time dependence of the fluorescence signals as a function of the buffer gas density the cross sections for quenching, fine structure transfer, and hyperfine structure transfer could be obtained. For N2 molecules the collisions can be described by a decoupling model as has been shown previously for the noble gases as collision partners.
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.