Intrinsic room-temperature ferromagnetism in a two-dimensional semiconducting metal-organic framework

Abstract The development of two-dimensional (2D) magnetic semiconductors remains a challenging issue in materials science, and plays an important role in the next-generation spintronics devices. Herein, we demonstrate that a 2D semiconducting antiferromagnetic Cu-MOF can be endowed with intrinsic room-temperature ferromagnetic coupling using a ligand cleavage strategy to regulate the inner magnetic interaction within the Cu dimers. Notably, employing the element-selective X-ray magnetic circular dichroism (XMCD) technique, we provide an unambiguous evidence for intrinsic ferromagnetism. Exhaustive structural characterizations confirm that the change of magnetic coupling is caused by the increased distance between Cu atoms within a Cu dimer. Theoretical calculations reveal that the ferromagnetic coupling is enhanced with the increased Cu-Cu distance, which depresses the hybridization between 3d orbitals of nearest Cu atoms. Our work provides an effective avenue to design and fabricate MOF-based semiconducting room-temperature ferromagnetic materials, and promotes their practical applications in next-generation spintronics devices.