Metal intercalation induced magnetic modulation in VS2 bilayers: a first principles study†

Abstract

Two-dimensional (2D) magnetic materials have emerged as highly promising candidates for spintronic applications owing to their unique properties. However, they tend to exhibit antiferromagnetic coupling when stacked, which limits their broader applications. It is of critical importance to manipulate the magnetic coupling and explore their applications in low-energy-consumption spintronic devices. Here, we theoretically investigated the electronic and magnetic properties of VS₂ bilayers intercalated with transition metals (TMs) using density functional theory (DFT) computations and the nonequilibrium Green's function (NEGF) method. It is revealed that metal intercalation can significantly enhance the ferromagnetic exchange interaction. The TM-intercalated VS₂ bilayers (TM–VS₂) exhibit diverse electronic and magnetic properties, which can be precisely tuned via controlling the type and concentration of intercalated metals. The spin-polarized transport calculations demonstrate that the TM–VS₂ bilayer with half-metallicity exhibits pronounced spin filtering properties. Our theoretical study provides a promising route to design and modulate the magnetic properties of 2D ferromagnets for their applications in advanced spintronic devices.