Nitrogen Enables the Intensity Modulation of Charge Transfer and Spin Paramagnetism in Graphdiyne

The modulation of intrinsic properties, including magnetism in two-dimensional materials, has attracted considerable interest as it expands device performance and allows for advanced flexible electronics. Herein, a facile way is developed to modulate the magnetic and electrical response of graphdiyne (GDY) by precise nitrogen doping. The introduced nitrogen exists only in the form of specific pyridine nitrogen and can meet the relative change of 1:2:3 between different materials, which can be used as a switch-like property to manipulate charge transfer and spin. Among these, triazine-graphdiyne (TA-GDY) with the most nitrogen content achieves the highest saturation magnetization of up to 3.0 emu/g at 2 K. The accompanying moderate band gap and mobility of up to 7.56 cm2·V–1·s–1 endow it a broad application prospect. These results revealed that controllable nitrogen doping can modulate the physical properties of carbon-based materials, thus providing a critical way to extend their application in future carbon electronics involving spin.