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Magneto-ionics has emerged as a promising approach to manipulate magnetic properties, not only by drastically reducing power consumption associated with electric current based devices but also by enabling novel functionalities. To date, magneto-ionics have been mostly explored in oxygen-based systems, while there is a surge of interest in alternative ionic systems. Here we demonstrate highly effective hydroxide-based magneto-ionics in electrodeposited α-Co(OH) 2 films. The α-Co(OH) 2 , which is a room temperature paramagnet, is switched to ferromagnetic after electrolyte gating with a negative voltage. The system is fully, magnetically reversible upon positive voltage application. The origin of the reversible paramagnetic-to-ferromagnetic transition is attributed to the ionic diffusion of hydroxyl groups, promoting the formation of metallic cobalt ferromagnetic regions. Our findings demonstrate one of the lowest turn-on voltages reported for propylene carbonate gated experiments. By tuning the voltage magnitude and sample area we demonstrate that the speed of the induced ionic effect can be drastically enhanced. 

The magnetic properties of cobalt metal nanowires grown by electrodeposition in porous membranes depend largely on the synthesis conditions. Here, we focus on the role of electrolyte additives on the magnetic anisotropy of the electrodeposited nanowires. Through magnetometry and internal field nuclear magnetic resonance (IF NMR) studies, we compared both the magnetic and crystalline structures of 50 and 200 nm diameter Co nanowires synthesized in the presence or absence of organic additives. The spectral characteristics of IF NMR were compared structurally to X-ray diffraction patterns, and the anisotropy of the NMR enhancement factor in ferromagnetic multidomain structures to magnetometry results. While the magnetic behavior of the 50 nm nanowires was dominated, as expected, by shape anisotropy with magnetic domains oriented on axis, the analysis of the 200 nm proved to be more complex. 59 Co IF NMR revealed that the determining difference between the samples electrodeposited in the presence or in absence of organic additives was not the dominant crystalline system (fcc or hcp) but the coherent domain sizes and boundaries. In the presence of organic additives, the cobalt crystal domains are smaller and with defective grain boundaries, as revealed by resonances below 210 MHz. This prevented the development in the Co hcp part of the sample of the strong magnetocrystalline anisotropy that was observed in the absence of organic additives. In the presence of organic additives, even in nanowires as wide as 200 nm, the magnetic behavior remained determined by the shape anisotropy with a positive effective magnetic anisotropy and strong anisotropy of the NMR enhancement factor. 

Magnetic skyrmions are topologically nontrivial spin textures with envisioned applications in energy-efficient magnetic information storage. Toggling the presence of magnetic skyrmions via writing/deleting processes is essential for spintronics applications, which usually require the application of a magnetic field, a gate voltage or an electric current. Here we demonstrate the reversible field-free writing/deleting of skyrmions at room temperature, via hydrogen chemisorption/desorption on the surface of Ni and Co films. Supported by Monte-Carlo simulations, the skyrmion creation/annihilation is attributed to the hydrogen-induced magnetic anisotropy change on ferromagnetic surfaces. We also demonstrate the role of hydrogen and oxygen on magnetic anisotropy and skyrmion deletion on other magnetic surfaces. Our results open up new possibilities for designing skyrmionic and magneto-ionic devices.

 

Abstract Magneto-ionics, understood as voltage-driven ion transport in magnetic materials, has largely relied on controlled migration of oxygen ions. Here, we demonstrate room-temperature voltage-driven nitrogen transport ( i.e ., nitrogen magneto-ionics) by electrolyte-gating of a CoN film. Nitrogen magneto-ionics in CoN is compared to oxygen magneto-ionics in Co 3 O 4 . Both materials are nanocrystalline (face-centered cubic structure) and show reversible voltage-driven ON-OFF ferromagnetism. In contrast to oxygen, nitrogen transport occurs uniformly creating a plane-wave-like migration front, without assistance of diffusion channels. Remarkably, nitrogen magneto-ionics requires lower threshold voltages and exhibits enhanced rates and cyclability. This is due to the lower activation energy for ion diffusion and the lower electronegativity of nitrogen compared to oxygen. These results may open new avenues in applications such as brain-inspired computing or iontronics in general.