Two-dimensional rare-earth Janus 2$\textit{H}$-Gd$\textit{XY}$ ($\textit{X}$,$\textit{Y}$=Cl, Br, I, $\textit{X}$$\neq$$\textit{Y}$) monolayers: Bipolar ferro-magnetic semiconductors with high Curie temperature and large valley polarization

Abstract

Two-dimensional (2D) ferromagnetic semiconductors show great interest due to their potential applications for the nanoscale electronic devices. In this work, the Janus 2$H$-Gd$XY$ ($X$, $Y$=Cl, Br, I, $X$$\neq$$Y$) monolayers with rare-earth element Gd (4$f^{7}$+5$d^{1}$) are predicted by the first-principles calculations. Small exfoliation energy of less than 0.25 J/m$^{2}$ and excellent dynamical/thermal stabilities can be confirmed for the Janus 2$H$-Gd$XY$ monolayers, which exhibit the bipolar magnetic semiconductor character with high Curie temperatures above 260 K and large spin-orbit coupling effect, and can be further transformed into the half-semiconductor phase under proper tensile strains (5-6\%). In addition, the in-plane magnetic anisotropy can be observed in the 2$H$-GdICl and 2$H$-GdIBr monolayers. On the contrary, the 2$H$-GdBrCl monolayer exhibits perpendicular magnetic anisotropy character, which originates from the competition between Gd-$p$/$d$ and halogen atom-$p$ orbitals. Calculated valley optical actions of the Janus 2$H$-Gd$XY$ monolayers exhibit distinguished valley-selective circular dichroisms, which is expected to realize the special valley excitation by polarized light. Spontaneously valley-Zeeman effect in the valance band for the Janus 2$H$-Gd$XY$ monolayers induces a giant valley splitting of 60-120 meV, which is also robust against various external biaxial strains. Tunable valley degree of freedom in the Janus 2$H$-Gd$XY$ systems is very necessary for encoding and processing information.