Tunable band gap and enhanced ferromagnetism by surface adsorption in monolayer Cr2Ge2Te6

Abstract

Two-dimensional (2D) van der Waals (vdW) materials have attracted significant attention for their promising applications in spintronic devices. Here, using first-principles calculations and renormalized spin-wave theory, we investigate the influence of surface adsorption (H and alkali metals) on the bandgap and ferromagnetism of monolayer ${\mathrm{Cr}}_{2}{\mathrm{Ge}}_{2}{\mathrm{Te}}_{6}$. We find that H-atom adsorption maintains the bandgap of ${\mathrm{Cr}}_{2}{\mathrm{Ge}}_{2}{\mathrm{Te}}_{6}$ around 0.95 eV but leads to a nearly indirect-to-direct band gap transition, while alkali-metal adsorption removes the bandgap and induces metallicity. More importantly, both H and alkali-metal adsorption surprisingly make the magnetic anisotropy energy four times larger than that of pristine ${\mathrm{Cr}}_{2}{\mathrm{Ge}}_{2}{\mathrm{Te}}_{6}$, leading to an increase of ${T}_{\mathrm{c}}$ by about 33%. Our findings of adsorption-controlled bandgap and magnetism in a 2D vdW magnet may open up opportunities for potential applications for new-generation magnetic memory storage, sensors, and spintronics.