Frustrated\nMagnetism in a Gyroidal Metal–Organic\nFramework Magnet

Metal–organic frameworks (MOFs) present a diverse\nchemical\nplatform, leading to innovative breakthroughs in functional materials\ndue to their controllable properties. In recent years, significant\nprogress has been made in the realm of MOF magnets, with a primary\nemphasis on developing new molecule-based magnets for various applications.\nNevertheless, the potential of MOFs as a platform for understanding\nquantum magnetism is still cultivating. Herein, based on detailed\nhigh-magnetic-field experiments on single crystals of Co(II)-oxalate\ngyroidal MOF, we revealed the competition of multiple quantum magnetic\nstates. Although such phase competition is typically observed in geometrically\nfrustrated magnets, the gyroidal structure does not inherently induce\ngeometric frustration for spins. We propose that in this system, the\nemergence of bond-dependent anisotropic interactions and tilting of\nthe local trigonal axis lead to the observed competition. This finding\nunveils the potential of MOF magnets as a novel source of quantum\nmagnetism.