Abstract
The concepts of bond orbitals and unrestricted Hartree-Fock orbitals are used in an attempt to explain the mechanism of superexchange between magnetic cations via an intermediate anion. The resulting theory predicts the same results as the standard theories when the cation-anion-cation angle is 180°. For other values of this angle, however, the nature and strength of the interaction depends on the distribution of bonds round the anion and is not solely a function of angle. The theory is applied to compounds having the corundum-ilmenite and spinel structures, where it correlates the magnetic structures and transition temperatures for a number of compounds and enables these properties to be predicted for others.
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