THEORETICAL STUDIES OF FINE STRUCTURE IN THE GROUND STATE OF $O_{2}$

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1972

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Ohio State University

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The fine-structure constant $\lambda = \lambda_{ss} + \lambda_{so}$ in the ground $(^{3}{\Sigma}_{g}^{-})$, state of $O_{2}$ has been investigated with ab initio methods. Extensive configuration interaction (CI) calculations as a function of Slater basis-set refinement were carried out on the first-order spin-spin contribution $\lambda_{ss}$. The significance of various types of $\sigma^{-}$ and $\pi^{-}$ valence excitations were examined. It is found that although certain configurations beyond the Hartree-Fock model change the spin-spin parameter drastically, the net effect of CI tends to be self-cancelling. Less than half of the total splitting is attributable to $\lambda_{ss}$. The remaining part presumably arises from the second-order spin-orbit and spin-other-orbit terms $\lambda_{so}$. The excited states which couple with the ground-state via this mechanism have been studies in a preliminary way. Their importance will be compared and discussed with reference to the experimental data.

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Author Institution: Battelle Memorial Institute; Department of Chemistry, The Ohio State University

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