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Four new compounds of formulas [Cu(hfac) 2 (L)] ( 1 ), [Ni(hfac) 2 (L)] ( 2 ), [{Cu(hfac) 2 } 2 (µ-L)]·2CH 3 OH ( 3 ) and [{Ni(hfac) 2 } 2 (µ-L)]·2CH 3 CN ( 4 ) [Hhfac = hexafluoroacetylacetone and L = 3,6-bis(picolylamino)-1,2,4,5-tetrazine] have been prepared and their structures determined by X-ray diffraction on single crystals. Compounds  1  and  2  are isostructural mononuclear complexes where the metal ions [copper(II) ( 1 ) and nickel(II) ( 2 )] are six-coordinated in distorted octahedral MN 2 O 4  surroundings which are built by two bidentate hfac ligands plus another bidentate L molecule. This last ligand coordinates to the metal ions through the nitrogen atoms of the picolylamine fragment. Compounds  3  and  4  are centrosymmetric homodinuclear compounds where two bidentate hfac units are the bidentate capping ligands at each metal center and a bis-bidentate L molecule acts as a bridge. The values of the intramolecular metal···metal separation are 7.97 ( 3 ) and 7.82 Å ( 4 ). Static (dc) magnetic susceptibility measurements were carried out for polycrystalline samples  1 – 4  in the temperature range 1.9–300 K. Curie law behaviors were observed for  1  and  2 , the downturn of χ M  T  in the low temperature region for  2  being due to the zero-field splitting of the nickel(II) ion. Very weak [ J  = −0.247(2) cm −1 ] and relatively weak intramolecular antiferromagnetic interactions [ J  = −4.86(2) cm −1 ] occurred in  3  and  4 , respectively (the spin Hamiltonian being defined as   H   = − J S   1 ·  S   2 ). Simple symmetry considerations about the overlap between the magnetic orbitals across the extended bis-bidentate L bridge in  3  and  4  account for their magnetic properties.

Mono- and Binuclear Copper(II) and Nickel(II) Complexes with the 3,6-Bis(picolylamino)-1,2,4,5-Tetrazine Ligand