EXPERIMENTAL AND THEORETICAL INVESTIGATION OF THE ELECTRONIC STRUCTURE OF CaF

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1978

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Ohio State University

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Optical-optical double resonance experiments on CaF have been performed using two cw dye lasers. The $E^{\prime}{^{2}\Pi} - A^{2}\Pi$ and $A^{2}\Pi - X^{2}\Sigma^{+}$ transitions are sequentially pumped by Rhodamine 110 and 6G dye lasers respectively. The $E^{\prime}{^{2}\Pi}$ state ($T_{0} \sim 34\; 490 cm^{-1}, B_{o} \sim 0.358\;cm^{-1}$) has not been observed previously and a vibration-rotation analysis is in progress. $E^{\prime}{^{2}\Pi} - B^{2}\Sigma^{+}$ fluorescence allows analysis of the $B^{2}\Sigma^{+}$ state [preliminary constants $T_{o} = 18 830(2) cm^{-1}, w_{e} = 571.5(5), w_{e} x_{3} = 3.0(2), B_{o} = 0.3439(5)\;cm^{-1}$. The differences between these constants and those in $Rosen^{1}$ are due to a large separation between bandheads and origins and to an error in the previous B-X rotational $analysis^{2}$ In addition, the double resonance fluorescence spectrum contains a cascade $Z-A^{2}\Pi$ transition. The Z state is either $^{2}\Sigma$ or $^{2}\Delta$ and has $T_{o} \sim 30 170\;cm^{-1}, B_{o} = 0.362\;cm^{-1}$. Semi-empirical and SCF-CI calculations of the electronic structure of CaF will be discussed with particular emphasis on the location on the lowest energy $^{2}\Delta$ state.

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$^{1}$B. Rosen (ed.), Spectroscopic Data Relative to Diatomic Molecules Pergamon 1970. $^{2}$D. P. Nanda and B. S. Mohanty, Curr. Sci. (India) 39, 300 (1970).""
Author Institution: Department of Chemistry, Massachusetts Institute of Technology; Laboratoire de Spectroscopie des Mol\'ecules Diatomiques, Universit\'e de Lille (I)

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