Owing to the unusual magnetic behaviors from the reduced dimensionality and frustration, low-dimensional magnetic systems attract considerable attention. Recently, we synthesized a heterometallic molecular tetramer compound [Cu(H2O)dmbpy]2[V2O2F8] (dmbpy = 4,4'-dimethyl-2,2'-bipyridyl) and single crystal X-ray diffraction reveals that the compound contains a triangular “CuV2” fragment with ordered oxide and fluoride ligands. This fragment is also observed in a reported spin-gapped chain compound [enH2]Cu(H2O)2[V2O2F8] (enH2 = ethylene diammonium). However, the triangular “CuV2” fragments in both compounds exhibit distinct Cu(II)−V(IV) superexchange interactions along two Cu−F−V pathways despite having similar bond angles. The strong disparity is found to originate from the specific orientation of the half-filled Cu dx2–y2 orbital stabilized by the crystal field that leads to different orbital overlaps along the two pathways. As a result, the magnetic behavior of the 0-D molecular tetramer and the 1-D chain compound is rationalized as that of weakly coupled spin dimers and spin trimers, respectively.

Designing low-dimensional magnetic systems with Cu(II)–V(IV) coupling

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