High temperature spin-polarized semiconductivity with zero magnetization in two-dimensional Janus MXenes

Abstract

Searching for two-dimensional (2D) materials with room-temperature magnetic order and high spin-polarization is essential for the development of next-generation nanospintronic devices. A new class of 2D magnetic materials with high Néel temperature, fully compensated antiferromagnetic order (zero magnetization) and completely spin-polarized semiconductivity is proposed for the first time. Based on the density functional theory calculations, we predict these properties for asymmetrically functionalized MXenes (Janus Cr₂C) – Cr₂CXX′ (X, X′ = H, F, Cl, Br, OH). The valence and conduction bands in these materials are made up of opposite spin channels and they can behave as bipolar magnetic semiconductors with zero magnetization. A Néel temperature as high as 400 K has been found for Cr₂CFCl, Cr₂CClBr, Cr₂CHCl, Cr₂CHF, and Cr₂CFOH materials. Remarkably, the spin carrier orientation and induced transition from bipolar magnetic semiconductors to half-metal antiferromagnets can be easily controlled by electron or hole doping. The band gap of Janus MXenes can be effectively tuned by the selection of a pair of chemical elements/functional groups terminating the upper and the lower surfaces. The spin-polarized semiconductivity with zero magnetism is preserved when MXenes are put on the SiC(0001) support. The results presented herein open a new road towards the construction of 2D high-temperature spin-polarized materials with antiferromagnetism potentially suitable for spintronic applications.