Chiral Supramolecular Nanotubes of Single‐Chain Magnets

We report a single‐chain magnet (SCM) made of a terbium(III) building block and a nitronyl‐nitroxide radical (NIT) functionalized with an aliphatic chain. This substitution is targeted to induce a long‐range distortion of the polymeric chain and accordingly it gives rise to chains that are curled with almost 20 nm helical pitch. They self‐organize as a chiral tubular superstructure made of 11 chains wound around each other. The supramolecular tubes have a 4.5 nm internal diameter. Overall, this forms a porous chiral network with almost 44 % porosity. Ab initio calculations highlight that each Tb III ion possesses high magnetic anisotropy. Indeed, notwithstanding the supramolecular arrangement each chain behaves as a SCM. Magnetic relaxation with both finite and infinite‐size regimes is observed and confirms the validity of the Ising approximation. This is associated with quite strong coercive field and magnetic remanence ( H c =2400 Oe M R =2.09 μ B at 0.5 K) for this class of compounds.