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A new dinuclear complex [{Fe(tpc-OBn)(NCS)(μ-NCS)} 2 ] (1) based on the tripodal tpc-OBn ligand (tpc-OBn = tris(2-pyridyl)benzyloxymethane), containing bridging μ-κN:κS-SCN and terminal κN-SCN thiocyanate ligands, has been prepared and characterized by single crystal X-ray diffraction, magnetic studies, and DFT theoretical calculations. This complex represents the first example of dinuclear Fe II complex with double μ-κN:κS-SCN bridges in a head-to-tail configuration that exhibits ferromagnetic coupling between metal ions (J FeFe = +1.08 cm -1 ). Experimental and theoretical magnetostructural studies on this kind of infrequent Fe II dinuclear complex containing a centrosymmetrically [Fe 2 (μ-SCN) 2 ] bridging fragment show that the magnitude and sign of the magnetic coupling parameter, J FeFe , depend to a large extent on the Fe-N-C (α) angle, so that J FeFe decreases linearly when α decreases. The calculated crossover point below which the magnetic interactions change from ferromagnetic to antiferromagnetic is found at 162.3°. In addition, experimental results obtained in this work and those reported in the literature suggest that large N ripodal -Fe II distances and bent N-bound terminal κN-SCN ligands favor the high spin state of the Fe II ions, while short N ripodal -Fe II distances and almost linear Fe-N-C angles favor a stronger ligand field, which enables the Fe II ions to show spin crossover (SCO) behavior.

inorganic chemistry

On the Magnetic Coupling and Spin Crossover Behavior in Complexes Containing the Head-to-Tail [FeII2(μ-SCN)2] Bridging Unit: A Magnetostructural Experimental and Theoretical Study