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Hyperfine Interaction and Chemical Bonding in MgH, CaH, SrH, and BaH Molecules

Vol: 54, Issue: 1
1971
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ESRspectra of MgF, CaF, SrF, and BaF molecules in their ground 2 Σ states were measured while trapped in solid neon and argon matrices at 4°K. g tensors and hyperfine structure (hfs) constants for interaction with 19F, and in the case of SrF and BaF, with 87Sr and 137Ba, were determined. In all cases less than 4% of the spin density is on the F atom, supporting the evidence for their extreme ionicity. The variation in the anisotropic character of the 19F hfs probably indicates a slight increase in covalency in the lighter molecules. The hf interaction with the metal nucleus is quite anisotropic, demonstrating that the unpaired s electron on the M+ ion actually has appreciable p and d character, i.e., that the spherical s electron orbit in the free M+ ion is highly distorted by the F− ion in the molecule. This was supported by an approximate variational calculation considering the F− ion as a point charge. A negative Δg⊥ for the MgF molecule indicates that the lowest-lying 2 Î state is regular, in support of Walker and Richards' reinterpretation of the λ-type doubling.

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