Voltage-controlled ON−OFF ferromagnetism at room temperature in a single metal oxide film

Electric-field-controlled magnetism can boost energy efficiency in widespread applications. However, technologically, this effect is facing important challenges: mechanical failure in strain-mediated piezoelectric/magnetostrictive devices, dearth of room-temperature multiferroics, or stringent thickness limitations in electrically charged metallic films. Voltage-driven ionic motion (magneto-ionics) circumvents most of these drawbacks while exhibiting interesting magnetoelectric phenomena. Nevertheless, magneto-ionics typically requires heat treatments and multicomponent heterostructures. Here we report on the electrolyte-gated and defect-mediated O and Co transport in a Co₃O₄ single layer which allows for room-temperature voltage-controlled ON-OFF ferromagnetism (magnetic switch) via internal reduction/oxidation processes. Negative voltages partially reduce Co₃O₄ to Co (ferromagnetism: ON), resulting in graded films including Co- and O-rich areas. Positive bias oxidizes Co back to Co₃O₄ (paramagnetism: OFF). This electric-field-induced atomic-scale reconfiguration process is compositionally, structurally, and magnetically reversible and self-sustained, since no oxygen source other than the Co₃O₄ itself is required. This process could lead to electric-field-controlled device concepts for spintronics