Engineering magnetic anisotropy and exchange couplings in double transition metal MXenes via surface defects

Two-dimensional (2D) materials have been experimentally proven to manifest almost all types of material properties observed in bulk materials. However, 2D magnetism was elusive until recently. In this work, we used an approach that synergistically uses density functional theory, and Monte Carlo methods to investigate the magnetic and electronic properties of magnetic double transition metal MXene alloys (Hf₂MnC₂O₂and Hf₂VC₂O₂) by exploiting realistic surface terminations via creating surface defects including oxygen vacancies and H adatoms. We found that introducing surface oxygen vacancies or hydrogen adatoms is able to modify the electronic structures, magnetic anisotropies, and exchange couplings. Depending on the defect concentration, a ferromagnetic half-metallic state can be realized for both Hf₂VC₂O₂and Hf₂MnC₂O₂. Bare Hf₂VC₂O₂exhibits easy-axis anisotropy, whereas bare Hf₂MnC₂O₂exhibits easy-plane anisotropy; however, defects can change the latter to easy-axis anisotropy, which is preferable for spintronics applications. The considered defects were found to modify the magnetic anisotropy by as much as 300%. Defects also produce an inhomogeneous pattern of exchange couplings, which can further enhance the Curie temperature. In particular, Hf₂MnC₂O₂H_0.22was predicted to have a Curie temperature of about 171 K due to a combination of easy-axis anisotropy and a connected network of enhanced exchange couplings. Our calculations suggest a route toward engineering exchange couplings and magnetic anisotropy to improve magnetic properties.