Purely organic ferromagnets are rare, the main problem being the relative orientation of the spins in a three-dimensional network. The first example of ferromagnetic ordering in an imino-nitroxide radical is reported. A detailed analysis of the structure reveals that CCHO hydrogen bonds are responsible for both the crystal packing and the ferromagnetic spin interactions within an infinite chain of ordered molecules. This radical is unique: its structure is the first demonstration of the use of terminal acetylenes to generate supramolecular networks.
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