Space‐Charge Control of Magnetism in Ferromagnetic Metals: Coupling Giant Magnitude and Robust Endurance

Abstract Ferromagnetic metals show great prospects in ultralow‐power‐consumption spintronic devices, due to their high Curie temperature and robust magnetization. However, there is still a lack of reliable solutions for giant and reversible voltage control of magnetism in ferromagnetic metal films. Here, a novel space‐charge approach is proposed which allows for achieving a modulation of 30.3 emu/g under 1.3 V in Co/TiO 2 multilayer granular films. The robust endurance with more than 5000 cycles is demonstrated. Similar phenomena exist in Ni/TiO 2 and Fe/TiO 2 multilayer granular films, which shows its universality. The magnetic change of 107% in Ni/TiO 2 underlines its potential in a voltage‐driven ON–OFF magnetism. Such giant and reversible voltage control of magnetism can be ascribed to space‐charge effect at the ferromagnetic metals/TiO 2 interfaces, in which spin‐polarized electrons are injected into the ferromagnetic metal layer with the adsorption of lithium‐ions on the TiO 2 surface. These results open the door for a promising method to modulate the magnetization in ferromagnetic metals, paving the way toward the development of ionic‐magnetic‐electric coupled applications.