Multiple Orbital Effects and Magnetic Ordering in a Neutral Radical

This is the authors' abstract. We don't add key points for this paper.

The alternating ABABAB π-stacked architecture of the EtCN solvate of the iodo-substituted, oxobenzene-bridged bisdithiazolyl radical IBBO (space group Pnma) gives rise to strong ferromagnetic exchange along the π-stacks, and the material orders as a spin-canted antiferromagnet with T(N) = 35 K, with a spontaneous (canted) moment M(spont) = 1.4 × 10(-3) μB and a coercive field H(c) = 1060 Oe (at 2 K). The observation of spin-canting can only be understood in terms of multiorbital contributions to both isotropic and anisotropic exchange interactions, the magnitude of which are enhanced by spin-orbit effects arising from the heavy-atom iodine substituent. Pseudodipolar interactions lead to a net canted moment along the c-axis, while the sublattice magnetization is predicted to possess an easy a-axis.