Cooperativity in Organic Spin Materials and their Hybrid Systems: Steering of Magnetic Properties by Orientation of Radicals (B11)

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The project aims at designing, preparing, and characterizing novel purely organic spin systems, with the objective of realizing and maximizing ferromagnetic exchange couplings. While cooperative magnetic systems have been mostly realized by trial-and-error, our approach will be guided by predictive theoretical chemistry. The strength of magnetic exchange couplings will be maximized by optimizing the molecular building blocks, using thioxoverdazyls as well as symmetric and non-symmetric biradical systems and their mutual orientations. Further approaches will include the assembly of building blocks within porous inorganic host materials, the topochemical polymerization of verdazyl substituted polydiacetylenes and the design of polyverdazyl systems. Cooperative magnetism will be examined by temperature dependent magnetic susceptibility and field dependent magnetization measurements. Modern solid-state NMR and EPR experiments will be used to characterize these materials structurally and to investigate the strengths of intermolecular magnetic exchange interactions.