Measurements of the spin-Hamiltonian parameters of pairs of interacting T m 2 +ions in CaF,, SrF, and BaF, are described. Superexchange and magnetic dipole-dipole interactions are shown to be of comparable magnitude and the superexchange is highly anisotropic. As Tm2+ has a single hole in the 4f shell, in alkaline-earth iluorides it is at a site of high symmetry, and as so much is known about the system, the possibility that these systems are ideal for quantitative tests of superexchange theories is examined. In particular the applicability of the overlap model, which i s discussed in the following paper, is examined. It is suggested that the g-values indicate small lattice distortions which change the surroundings of the Tm2+ ion but preserve the D,, symmetry of the nearest-neighbour pair. This renders quantitative calculation of 'overlap' somewhat uncertain. However, within this limitation, several aspects of the interaction are consistent with the overlap model, but the model does not explain the anisotropy of the interaction. It is suggested that this is because of a major contribution from potential exchange which is not adequately described by the overlap model.