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New magnetic metal complexes with organic radical ligands, [M(hfac) 2 (PyBTM) 2 ] (M = Ni II , Co II ; hfac = hexafluoroacetylacetonato, PyBTM = (3,5-dichloro-4-pyridyl)bis(2,4,6-trichlorophenyl)methyl radical), were prepared and their crystal structures, magnetic properties, and electronic structures were investigated. Metal ions in [M(hfac) 2 (PyBTM) 2 ] constructed distorted octahedral coordination geometry, where the two PyBTM molecules ligated in the trans configuration. Magnetic investigation using a SQUID magnetometer revealed that χT increased with decreasing temperature from 300 K in the two complexes, indicating an efficient intramolecular ferromagnetic exchange interaction taking place between the spins on PyBTM and M with J/k  B of 21.8 K and 11.8 K for [Ni II (hfac) 2 (PyBTM) 2 ] and [Co II (hfac) 2 (PyBTM) 2 ]. The intramolecular ferromagnetic couplings in the two complexes could be explained by density functional theory calculations, and would be attributed to a nearly orthogonal relationship between the spin orbitals on PyBTM and the metal ions. These results demonstrate that pyridyl-containing triarylmethyl radicals are key building blocks for magnetic molecular materials with controllable/predictable magnetic interactions.

Structural and Magnetic Studies on Nickel(II) and Cobalt(II) Complexes with Polychlorinated Diphenyl(4-pyridyl)methyl Radical Ligands