Room-Temperature Ferromagnetism in Sulfur-Doped Graphdiyne Semiconductors

The realization of magnetic ordering in a two-dimensional graphitic semiconductor, graphdiyne, has attracted great interest because of its promising potential application in semiconductor devices involving spin. Here, we propose a simple and feasible sulfuration strategy to induce robust ferromagnetic ordering into graphdiyne and realize the coexistence of room-temperature ferromagnetism and semiconductivity in graphdiyne without extrinsic magnetic impurity. The robust residual magnetization of more than 0.047 emu g(-1) at room temperature and transition temperature of up to 460 K indicate great potential for application in magnetic storage. The subsequent spin-polarized density functional theory calculation reveals that the intrinsic ferromagnetic ordering originates from the enhanced local magnetic moment and nonlocal electron transfer between carbon atoms and sulfur atoms, which is well confirmed in our electrical measurements. This synthetic strategy could spur studies of two-dimensional magnetic semiconductors based on graphdiyne and even accelerate the potential application of graphdiyne in spintronic devices.