Abstract
The theory of spin-lattice relaxation is developed for S-state ions: in particular for Mn2+ in a cubic environment. The wavefunctions for Mn2+ are generated to first order in the spin-orbit coupling parameter, the orbit-lattice interaction is formulated in terms of spherical harmonics, and the rate equations are derived for this system. Estimates are given of the interaction coefficients based on a point-charge model, and it is shown that excellent agreement is obtained with observed spin-lattice relaxation times. However, a detailed comparison with recent experiments which give the magnitude and sign of these coefficients directly shows that though the point-charge model gives the right order of magnitude, it gives the wrong sign for the interaction coefficients.

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