Enhancing Magneto-Ionic Effects in Magnetic Nanostructured Films via Conformal Deposition of Nanolayers with Oxygen Acceptor/Donor Capabilities

Effective manipulation of the magnetic properties of nanostructured metallic alloys, exhibiting intergrain porosity (i.e., channels) and conformally coated with insulating oxide nanolayers, with an electric field is demonstrated. Nanostructured Co–Pt films are grown by electrodeposition (ED) and subsequently coated with either AlOx or HfOx by atomic layer deposition (ALD) to promote magneto-ionic effects (i.e., voltage-driven ion migration) during electrolyte gating. Pronounced variations in coercivity (HC) and magnetic moment at saturation (mS) are found at room temperature after biasing the heterostructures. The application of a negative voltage results in a decrease of HC and an increase of mS, whereas the opposite trend is achieved for positive voltages. Although magneto-ionic phenomena are already observed in uncoated Co–Pt films (because of the inherent presence of oxygen), the ALD oxide nanocoatings serve to drastically enhance the magneto-ionic effects because of partially reversible oxygen migration, driven by voltage, across the interface between AlOx or HfOx and the nanostructured Co–Pt film. Co–Pt/HfOx heterostructures exhibit the most significant magneto-electric response at negative voltages, with an increase of mS up to 76% and a decrease of HC by 58%. The combination of a nanostructured magnetic alloy and a skinlike insulating oxide nanocoating is shown to be appealing to enhance magneto-ionic effects, potentially enabling electrolyte-gated magneto-ionic technology.Financial support by the European Research Council (SPIN-PORICS 2014-Consolidator Grant, agreement no. 648454), the Spanish Government (Project MAT2017-86357-C3-1-R, MAT2017-83169-R “Severo Ochoa” Programme for Centres of Excellence in R&D SEV-2015-0496 and associated FEDER), the Generalitat de Catalunya (2017-SGR-292 and 2017-SGR-1519), and the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement no. 665919 is acknowledged. P.Y. acknowledges the Chinese Scholarship Council CSC fellowship (201606920073).Peer reviewe