ELECTRONIC STRUCTURE OF THE $B^{2}\sum^{+}, A^{2}\Pi$ AND $X^{2}\Sigma^{+}$ STATES OF THE CALCIUM MONOHALIDES

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1981

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Ohio State University

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The CaX molecules are the alkali atoms of diatomic molecular spectroscopy. The electronic transitions of these ionic radicals occur between singly-occupied, non-bonding metal-centred molecular orbitals. The molecular parameters are direct probes of the orbital character. A simple quantitative semi-empirical model will be described. This model provides an explanation for almost all of the known spectroscopic constants of the X, A and B states, including A-doubling, spin-rotation, spin-orbit, and lifetime and hyperfine constants. The hydrogenic model indicates that the $X^{2}\Sigma^{+}$ state is about 75% 4s$\sigma(Ca^{+}$) and 25 % 4p$\sigma(Ca^{+})$ while the $B^{2}\Sigma^{+}$ state is about 60% 4p$\sigma(Ca^{+})$ and 40% 3d$\sigma(Ca^{+})$ for the entire CaX series. The $A^{2}\Pi$ state is almost pure 4p$\pi$ in CaF (91%), but becomes increasingly mixed with 3d$\pi$ along the CaX series until for CaI the A state is only 70% 4p$\pi$.

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