Emergence of half-semiconductor behavior and tunable magnetism via carrier doping in Janus VXSe (X=Cl, Br, I) monolayers

Abstract

Two-dimensional ferromagnetic semiconductors with high Curie temperature, large magnetic anisotropy, and electrically tunable properties are highly sought for nanoscale spintronics. Here, using first-principles calculations, we predict a new class of Janus VXSe (X=Cl, Br, I) monolayers. All three compounds are intrinsic ferromagnetic semiconductors with indirect band gaps of 1.66-2.33 eV, Curie temperatures up to 128 K, and magnetic anisotropy energies up to 910 ueV per V, leading to easy-plane magnetization for VClSe and VBrSe and an out-of-plane easy axis for VISe. The robust ferromagnetic order originates from the competition between superexchange and itinerant magnetism. Remarkably, VISe is a pristine half-semiconductor, whereas carrier doping unlocks fully spin-polarized states in the initially non-ideal VClSe and VBrSe. We also find that hole doping can switch the magnetic easy axis of VBrSe from in-plane to out-of-plane, enabling a spin-field-effect transistor with giant magnetoresistance. Our findings highlight carrier doping as a key to unlock hidden half-semiconducting behavior and establish Janus VXSe as a promising platform for 2D spintronics and magnetoelectric devices.