This paper presents a detailed study of the solid-state chemical, spectral, structural, and charge transport properties of the materials which result from treating nickel phthalocyanine (NiPc) with elemental iodine. A range of NiPcI* stoichiometries is obtained where x = 0 to ca. 3.0; electrical conductivities of compressed polycrystalline samples are comparable with those of other "molecular metals". Single crystals were obtained for NiPcI10. These crystallize in the space group D^-PA/mcc,

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A complete treatment of the spin hamiltonian for a pair of exchange coupled metal ions is given. The results obtained through the use of the Wigner-Eckart theorem are unrestricted with respect to the relative orientation of the single-ion tensors, and appropriate for both the S1 = $2 and 314 32 cases. The necessary constants are derived so that matrix elements within a given spin multiplet can be treated by ordinary operator algebra with the coupled representation state vectors, I SM), as a basis set. Explicit algebraic formulae for matrix elements between spin multiplets are presented for the first time. Symmetry restrictions are discussed in general and illustrated for the simple case of two ions related by an inversion centre, pair symmetry Ci.