Published online by Cambridge University Press: 25 February 2011
The temperature dependence of the magnetic susceptibilities for several ±-nitronyl nitroxides have been measured. It is found that the intermolecular magnetic coupling in these radical crystals changes from antiferromagnetic to ferromagnetic depending on the substituents at ±-position. X-Ray crystal analysis and MO calculation have been carried out on the ferromagnetic ±-nitronyl nitroxide, 2-(4-nitrophenyl)-4,4,5,5-tetramethyl-4,5-dihydro-1H-imidazolyl-1-oxy 3-oxide, revealing a two-dimensional ferromagnetic network linked by the Nδ+...0δ− Coulomb attraction.