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Multiferroicity and magnetodielectric coupling in metal-organic-frameworks(MOFs) is rare and so far restricted mainly to formate-based systems withperovskite structure. In the course of this work we designed a tetragonalframework [Co(C16H15N5O2)], exhibiting spin-chains of Co2+ ions, which arebridged by an organic linker containing a dipolar nitrobenzene moiety. Thiscompound shows relaxor-like ferroelectricity at 100 K, which is followed by theonset of complex magnetic order at 15 K, indicative of weak ferromagnetism. Theclear anomaly of the dielectric constant at the magnetic ordering transitionindicates magnetodielectric coupling, which is also confirmed by magnetic-fielddependent dielectric measurements. Weak ferromagnetism and magnetodielectriccoupling, both probably result from a significant Dzyaloshinskii-Moriyainteraction, which cants the spin structure and locally breaks inversionsymmetry. We document that the introduction of dipolar nitrobenzene as buildingblock in the crystal structure paths the way to design new multiferroic andmagnetodielectric MOFs.

Magnetodielectric coupling in a non-perovskite metal-organic framework