Abstract

The solid state magnetic properties of a series of tert-butylnitroxides are compared: benzimidazole-2- tert-butylnitroxide (BImtBN), 4-(1H-benzimidazol-2-yl-phenyl- tert-butyl-nitroxide (BImPhtBN), 5(6)-chloro-BImtBN, and 5,6-dimethyl-BImtBN, ( 1– 4, respectively). The series shows decreasing crystallographic unit cell complexity and increasing simplicity of magnetic behavior: 1– 2 show magnetic behavior that has a good fit to a 2D simple planar Heisenberg AFM model, and 3– 4 show Bleaney–Bowers dimeric AFM exchange behavior. Hydrogen bonding in 3– 4 appears to play a crystallographic assembly — rather than an electronic exchange — role in the magnetic behavior of these systems.

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