Abstract Secondary hydrogen-bonding interactions have been exploited to construct layered magnetic solids based on amidinium–carboxylate salt bridges. The salt bridge is utilized as a supramolecular synthon to set the structural organization in a layered motif; it also serves as a spin communication element. The magnetic material shown in the accompanying figure is formed between 3-cyanobenzamidinium and 2, 2, 4, 4-tetramethylpyrroline-N-oxyl-3- ...
