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

Feng Sihua,Duan Hengli,Tan Hao,Hu Fengchun,Liu Chaocheng,Wang Yao,Li Zhi,Cai Liang,Cao Yuyang,Wang Chao,Qi Zeming,Song Li,Liu Xuguang,Sun Zhihu,Yan Wensheng

The development of two-dimensional (2D) magnetic semiconductors with room-temperature ferromagnetism is a significant challenge in materials science and is important for the development of next-generation spintronic 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. Using the element-selective X-ray magnetic circular dichroism (XMCD) technique, we provide 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 3 d 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 spintronic devices.