Abstract
Long-range ferrimagnetic order in which one magnetic sub-lattice is formed from partly-occupied p-orbitals and the other from d-orbitals can be achieved in molecular ion-radical salts where the cations are oxidised organo-chalcogen donors and the anions are 3d-metal complexes containing both N-bonded NCS and planar N-heterocyclic ligands. Overlaps between p-orbitals of the radical cations and those of the heterocycle are implicated in the cation-anion exchange pathway.