Tunable Half-metallic Magnetism in Atom-thin Holey Two-dimensional C${}_2$N Monolayer

Abstract

Exploring two-dimensional (2D) materials with magnetic ordering is a focus of current research. It remains a challenge to achieve tunable magnetism in a material of one-atom-thickness without introducing extrinsic magnetic atoms or defects. Here, based on first-principles calculations, we propose that tunable ferromagnetism can be realized in the recently synthesized holey 2D C${}_2$N ($h$2D-C${}_2$N) monolayer via purely electron doping that can be readily achieved by gating. We show that owing to the prominent van Hove singularity in the band structure, the material exhibits ferromagnetism even at a small doping level. Remarkably, over a wide doping range of 4$\times$10${}^{13}$/cm${}^2$ to 8$\times$10${}^{13}$/cm${}^2$, the system becomes half-metallic, with carriers fully spin-polarized. The estimated Curie temperature can be up to 320 K. Besides gating, we find that the magnetism can also be effectively tuned by lattice strain. Our result identifies $h$2D-C${}_2$N as the first material with single-atom-thickness that can host gate-tunable room-temperature half-metallic magnetism, suggesting it as a promising platform to explore nanoscale magnetism and flexible spintronic devices.

12 pages, 5 figures

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• Robust p-orbital half-metallicity and high Curie-temperature in the hole-doped anisotropic TcS2 (X=S, Se) nanosheets
• Combined sub-sampling and analytical integration for efficient large-scale $GW$ calculations for 2D systems