Monolayer CeI2 : An intrinsic room-temperature ferrovalley semiconductor

Abstract

Two-dimensional ferrovalley semiconductors with robust room-temperature ferromagnetism and sizable valley polarization hold great prospects for future miniature information storage devices. As a new member of the ferroic family, however, such ferrovalley materials have rarely been reported. By first-principles calculations, we identify that monolayer $\mathrm{Ce}{\mathrm{I}}_{\text{2}}$ is an intrinsic ferromagnetic semiconductor and exhibits excellent ambient stability, strong easy in-plane magnetocrystalline anisotropy, and a high magnetic transition temperature up to 374 K. The ferromagnetism is found to arise from the hybridization of Ce-$4f/5d$ and I-$5p$ orbitals. When monolayer $\mathrm{Ce}{\mathrm{I}}_{\text{2}}$ is magnetized toward the off-plane $z$ direction, a spontaneous valley polarization as large as 208 meV in the top valence band can be achieved due to the simultaneous breaking of both inversion symmetry and time-reversal symmetry, which is further verified by the perturbation theory of spin-orbital coupling. Also, the anomalous valley Hall effect can be observed under an in-plane electrical field due to the robust valley-contrasting Berry curvature. Overall, the combination of intrinsic semiconducting ferromagnetism and spontaneous valley polarization renders monolayer $\mathrm{Ce}{\mathrm{I}}_{\text{2}}$ a compelling room-temperature ferrovalley semiconductor for potential applications in nanoscale spintronics and valleytronics.