Magnetic and electronic properties of two-dimensional metal-organic frameworks TM3(C2NH)12 * *Project supported by the National Natural Science Foundation of China (Grant Nos. 62074053, 61901161, 21906041, and 11774079), the Natural Science Foundation of Henan Province, China (Grant Nos. 202300410226, 202300410237, and 202300410100), Henan Overseas Expertise Introduction Center for Discipline Innovation (Grant No. CXJD2019005), and key scientific research projects of Colleges and

Abstract

The ferromagnetism of two-dimensional (2D) materials has aroused great interest in recent years, which may play an important role in the next-generation magnetic devices. Herein, a series of 2D transition metal-organic framework materials (TM-NH MOF, TM = Sc–Zn) are designed, and their electronic and magnetic characters are systematically studied by means of first-principles calculations. Their structural stabilities are examined through binding energies and ab-initio molecular dynamics simulations. Their optimized lattice constants are correlated to the central TM atoms. These 2D TM-NH MOF nanosheets exhibit various electronic and magnetic performances owing to the effective charge transfer and interaction between TM atoms and graphene linkers. Interestingly, Ni- and Zn-NH MOFs are nonmagnetic semiconductors (SM) with band gaps of 0.41 eV and 0.61 eV, respectively. Co- and Cu-NH MOFs are bipolar magnetic semiconductors (BMS), while Fe-NH MOF monolayer is a half-semiconductor (HSM). Furthermore, the elastic strain could tune their magnetic behaviors and transformation, which ascribes to the charge redistribution of TM-3d states. This work predicts several new 2D magnetic MOF materials, which are promising for applications in spintronics and nanoelectronics.