Nonvolatile ferroelectric control of both magnetic anisotropy and half-metallicity in multiferroic heterostructures GdI 2 /Al2Te3

Nonvolatile all-electric spin manipulation is optimal for low-power and compact spintronic devices. Herein, using first-principles density functional theory, we propose a bilayer van der Waals (vdW) multiferroic heterostructure (HS) GdI 2 /Al 2 Te 3 constructed of ferromagnetic electride GdI 2 and ferroelectric (FE) semiconductor Al 2 Te 3 to possess robust magnetoelectric coupling near room temperature. By reversing the electrical polarization states in Al 2 Te 3 , the magnetoelectric coupling not only allows the reversible switch of GdI 2 from semiconductor to half-metal but also promotes the reversible transition of magnetocrystalline anisotropy from in-plane to out-of-plane. More importantly, the high Curie temperature ( T C ) of GdI 2 and the unspoiled semiconducting nature of Al 2 Te 3 in the HS predict the practical feasibility of this spin manipulation. Additionally, GdI 2 exhibits substantial valley polarization when its magnetization direction changes to out-ofplane. These findings pave the way for achieving robust and efficient spin manipulation through all-electric control and also provide implications for multiferroic memory devices with highly efficient data reading and writing based on the HS.