Coexisting Magnetism, Ferroelectric, and Ferrovalley Multiferroic in Stacking-Dependent Two-Dimensional Materials

The two-dimensional (2D) multiferroic materials have widespread of application prospects in facilitating the integration and miniaturization of nanodevices. However, it is rarely coupling between the magnetic, ferroelectric, and ferrovalley in one 2D material. Here, we propose a mechanism for manipulating magnetism, ferroelectric, and valley polarization by interlayer sliding in 2D bilayer material. Monolayer GdI2 exhibits a ferromagnetic semiconductor with the valley polarization up to 155.5 meV. More interestingly, the magnetism and valley polarization of bilayer GdI2 can be strongly coupled by sliding ferroelectricity, appearing these tunable and reversible. In addition, we uncover the microscopic mechanism of magnetic phase transition by spin Hamiltonian and electron hopping between layers. Our findings offer a new direction for investigating 2D multiferroic in the implication for next-generation electronic, valleytronic, and spintronic devices.