Monolayer gadolinium halides, GdX2 (X = F, Cl, Br): intrinsic ferrovalley materials with spontaneous spin and valley polarizations

Abstract

Two-dimensional (2D) intrinsic ferrovalley semiconductors provide unprecedented opportunities to investigate valley physics as well as providing promising device applications due to their exceptional combination of spontaneous spin and valley polarizations. Here, we have predicted from first-principles calculations and Monte Carlo simulations that monolayers (MLs) GdX₂ are such extremely rare excellent materials. Apart from their robust stabilities energetically, dynamically, thermally, and mechanically, these 2D materials are found to be semiconducting intrinsic ferromagnets where the magnetic coupling is ascribed to 5d-electron-mediated 4f–4f exchange interactions. Moreover, MLs GdX₂ (X = F, Cl, Br) not only exhibit significant magnetic anisotropy energy of 351, 268, and 30 μeV per Gd, but also have a high Curie temperature of 300, 245, and 225 K, respectively. In particular, spontaneous valley polarization in three systems occurs due to the cooperative interplay between the spin–orbit coupling and magnetic exchange interactions, whose magnitude is as sizable as 55, 38, and 82 meV for MLs GdF₂, GdCl₂, and GdBr₂, respectively. Under the action of an in-plane longitudinal electrical field, the valley-contrasting Berry curvatures arising from the broken space-inversion and time-reversal symmetries in MLs GdX₂ could yield opposite transverse velocities of the carriers, giving rise to the occurrence of a spin-polarized anomalous valley Hall effect. Overall, these findings render 2D GdX₂ a class of promising candidate materials for experimental studies and practical spintronics and valleytronics applications.