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The e m . study of a single crystal of NN'-ethylenebis(acetylacetoneiminato)cobalt(ii)-doped NN'-ethylenebis-(acetylacetoneiminato)nickel(ii), [Co(acacen)] and [Ni(acacen)], is reported ; determination of the ground state of the cobalt complex was attempted. [Ni(acacen)] Is isomorphous with [Co(acacen)] as shown by a single-crystal structural determination : the doped crystals are orthorhombic. space group Pna2,. Z = 4, a = 12.1 8(1), b = 10.28(1), and c = 10.37(1). The equatorial principal axes of the g tensor were found to be almost parallel with the cobalt-ligand bond, rather than between these bonds, as expected.

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