Realization of Robust and Ambient-Stable Room-Temperature Ferromagnetism in Wide Bandgap Semiconductor 2D Carbon Nitride Sheets

Due to their weak intrinsic spin−orbit coupling and a distinct bandgap of 3.06 eV, 2D carbon nitride (CN) flakes are promising materials for next-generation spintronic devices. However, achieving strong room-temperature (RT) and ambientstable ferromagnetism (FM) remains a huge challenge. Here, we demonstrate that the strong RT FM with a high Curie temperature (TC) up to ∼400 K and saturation magnetization (Ms) of 2.91 emu/g can be achieved. Besides, the RT FM exhibits excellent air stability, with Ms remaining stable for over 6 months. Through the magneto-optic Kerr effect, Hall device, X-ray magnetic circular dichroism, and magnetic force microscopy measurements, we acquired clear evidence of magnetic behavior and magnetic domain evolutions at room temperature. Electrical and optical measurements confirm that the Co-doped CN retains its semiconductor properties. Detailed structural characterizations confirm that the single-atom Co coordination and nitrogen defects as well as C−C covalent bonds are simultaneously introduced into CN. Density functional theory calculations reveal that introducing C−C bonds causes carrier spin polarization, and spin-polarized carrier-mediated magnetic exchange between adjacent Co atoms leads to longrange magnetic ordering in CN. We believe that our findings provide a strong experimental foundation for the enormous potential of 2D wide bandgap semiconductor spintronic devices. © 2023 American Chemical Society.