Abstract
Four tetracoordinate Ni(II) complexes have been prepared, structurally characterized, and subjected to magnetometric studies. The complexes [Ni(PPh3)2(NCS)2], [Ni(dppp)(NCS)2], and [Ni(dppm)Br2] are planar and thus diamagnetic. The complex [Ni(biqu)Br2] is quasi-tetrahedral, with the geometry close to C2v symmetry, and paramagnetic. While on one side it resembles a prolate bisphenoid (the angle N-Ni-N = 83 deg), on the second side it mimics an oblate bisphenoid (Br-Ni-Br = 126 deg). It exhibits a zero-field splitting of the ground term 3A2 into three crystal-field multiplets that can be described by D and E parameters within the spin Hamiltonian formalism. The ab initio calculations confirm this interpretation; however, the evaluation of the spin-Hamiltonian parameters meets difficulties owing to the quasi-degeneracy of the electronic terms.
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