The first paramagnetic pentagonal-bipyramidal complex of Mo(iii) with a N3O2-type Schiff-base ligand was synthesized by the comproportionation reaction between Mo(ii) and Mo(iv) congeners. The complex has a low-spin (S = 1/2) ground state of MoIII(4d3) with double orbital degeneracy and unquenched orbital momentum, which result in strong Ising-type magnetic anisotropy.

A heptacoordinate complex [Mo(DAPBH)Cl] (HDAPBH is 1,1'-(pyridine-2,6-diyl)bis(ethan-1-yl-1-ylidene)dibenzohydrazine) has been synthesized and characterized structurally and magnetically. It exhibits a slightly distorted pentagonal bipyramidal geometry and reveals paramagnetic behaviour resulting from two unpaired electrons (S = 1) with large positive zero-field splitting (D = +50 cm) and pronounced temperature-independent paramagnetism.

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This article overviews the current state and prospects of the concept of advanced single-molecule magnets (SMMs) based on low-spin (S = 1/2) pentagonal-bipyramidal (PBP) 4d3 and 5d3 complexes with unquenched...

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