A SUPERSONIC MOLECULAR BEAM STUDY OF ISOTOPICALLY SUBSTITUTED CALCIUM MONOCYANIDE

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1993

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Ohio State University

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Recently we $reported^{1}$ the results of a high resolution optical Stark spectroscopic study of the $(0,0,0)-(0,0,0) A{^{2}}\Pi - X^{2}\Sigma$ band system of calcium isocyanide, CaNC. Although the optical spectra could be reduced using a conventional effective Hamiltonian operator, the spectroscopic parameters for the ``$^{\prime}A^{2}\Pi^{\prime}$'' state were physically unrealistic. Specifically, $B^{\ast}-B^{\prime}$ was too large, $D^{\prime}< 0$, and the A-doubling parameters were too large. It was postulated that these effects were a result of large Renner-Teller effects and/or a mis-assignment of the excited state. Here we report on the results of the rotational analysis of the $Ca^{15}NC$ and $CaN^{13}C$ isotopic forms. Similar to previous $studies^{1,2}$, a supersonic molecular beam sample was produced by skimming the products of a laser ablation (355nm, 5 mJ/pulse, 20 Hz)/ reaction $(5\%CH_{3}CN/Ar)$ source. The spectra were recorded at a resolution of 50 MHz (FWHM). The $X^{2}\Sigma$ state data fits to a standard model and produces bond lengths of: Ca-N, .227(9) nm; N-C, .115(9)nm. At the time of this submittal it has been impossible to get a satisfactory reduction of the excited state eigenvalues for the $Ca^{14}N^{12}C, Ca^{15}NC$ and $CaN^{13}C$ isotopic forms.

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1.T.C. Steimle, D.A. Fletcher, K.Y. Jung and C.T. Scurlock, J. Chem. Phys. 97, 2909 (1992). 2.C.J.Whitham, B.Soep, J-P. Visticot and A.Keller, J.Chem.Phys. 93, 991 (1990).
Author Institution: Department of Chemistry, Arizona State University

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