Materialization of a Geometrically Frustrated Magnetin a Hybrid Coordination Framework: A Study of the Iron(II) OxalateFluoride Framework, KFe(C 2 O 4 )F

Here we discuss magnetic hybrid coordination frameworks in relation to the realization of new geometrically frustrated magnets. In particular, we present the nuclear and magnetic structures of one such system—the Fe2+-based oxalate fluoride framework KFe(C2O4)F—through analysis of the powder neutron diffraction and muon spectroscopy data. KFe(C2O4)F retains an orthorhombic Cmc21 structure upon cooling to 2 K composed of quasi-one-dimensional iron fluoride chains connected to a distorted triangular network via oxalate anions. Previous magnetometry measurements of KFe(C2O4)F indicate that it is a strongly interacting system with a Weiss constant θ ≈ −300 K that undergoes a magnetic ordering transition at TN ≈ 20 K, yielding a frustration index, f = |θ|/TN ≈ 15, reflective of high-spin frustration. We determine the nature of this frustrated antiferromagnetic ordering below TN and show that the resulting magnetic structure is best described by a model in the Cmc′21′ magnetic space group.