Computational design of double transition metal MXenes with intrinsic magnetic properties

Abstract

Two-dimensional transition metal carbides (MXenes) have great potential to achieve intrinsic magnetism due to their available chemical and structural diversity. In this work, by spin-polarized density functional theory calculations, we designed and comprehensively investigated 50 double transition metal (DTM) MXenes MCr₂CT_x (T = H, O, F, OH, or bare) based on the chemical formula of M₂C (M = Sc, Y, Ti, Zr, Hf, V, Nb, Ta, Mo, W). We highlight that ferromagnetic half-metallicity, antiferromagnetic semiconduction, as well as antiferromagnetic half-metallicity have been achieved in the DTM MXenes. Herein, ferromagnetic half-metallic ScCr₂C₂, ScCr₂C₂H₂, ScCr₂C₂F₂, and YCr₂C₂H₂ are characterized with wide band gaps and high Curie temperatures. Very interestingly, the ScCr₂C₂-based magnetic tunnel junction presents a tunnel magnetoresistance ratio as high as 176 000%. In addition, the antiferromagnetic semiconducting TiCr₂C₂, ZrCr₂C₂, and ZrCr₂C₂(OH)₂, possessing moderate band gaps and high Néel temperatures, have been predicted. Especially, the Néel temperature of ZrCr₂C₂(OH)₂ can reach 425 K. Moreover, the Dirac cone-like band structure feature is highlighted in antiferromagnetic half-metallic ZrCr₂C₂H₂. Our study provides a new potential strategy for designing MXenes in spintronics.