Abstract
A mechanism for spin alignments in molecule-based ferrimagnets is proposed in terms of a Heisenberg spin Hamiltonian and molecular orbital calculations for a supramolecule composed of an S = 1 biradical and an S = 1/2 radical. Spin polarization in the supramolecule with an effective S = 1/2 spin is found to give ferromagnetic interactions between the supramolecules, leading to the ferrimagnetic ground state.
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