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.
Financial support by the European Research Council (SPINPORICS 2014-Consolidator Grant, Agreement No. 648454), the Spanish Government (Projects MAT2017-86357-C3-1-R and associated FEDER), the Generalitat de Catalunya (2017-SGR-292) and the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie Grant Agreement No. 665919 is acknowledged. E.P. is grateful to MINECO for the “Ramon y Cajal” contract (RYC-2012-10839). The ICN2 is funded by the CERCA programme/Generalitat de Catalunya. ICN2 also acknowledges the support from the Severo Ochoa Program (MINECO, Grant SEV-2013-0295). Work at UCD is supported by the US NSF (DMR1610060 and ECCS-1611424).