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Ferrimagnets have received renewed attention as a promising platform for spintronic applications. Of particular interest is the Mn4N from the ε-phase of the manganese nitride as an emergent rare-earth-free spintronic material due to its perpendicular magnetic anisotropy, small saturation magnetization, high thermal stability, and large domain wall velocity. We have achieved high-quality (001)-ordered Mn4N thin film by sputtering Mn onto η-phase Mn3N2 seed layers on Si substrates. As the deposited Mn thickness varies, nitrogen ion migration across the Mn3N2/Mn layers leads to a continuous evolution of the layers to Mn3N2/Mn2N/Mn4N, Mn2N/Mn4N, and eventually Mn4N alone. The ferrimagnetic Mn4N, indeed, exhibits perpendicular magnetic anisotropy and forms via a nucleation-and-growth mechanism. The nitrogen ion migration is also manifested in a significant exchange bias, up to 0.3 T at 5 K, due to the interactions between ferrimagnetic Mn4N and antiferromagnetic Mn3N2 and Mn2N. These results demonstrate a promising all-nitride magneto-ionic platform with remarkable tunability for device applications. 

Abstract Specific ions can be intercalated into functional materials using the electrolyte gating technique, which has been widely used to regulate channel conductance in transistors and develop low‐power neuromorphic devices. However, in these devices, fundamental exploration of ion intercalation‐induced structural phase transitions remains largely overlooked and rarely explored. Here, the lithium‐based electrolyte gating technique is used to probe the collective interactions between ions, lattices, and electrons in a van der Waals ferroelectric semiconductor α‐In₂Se₃. Using a polymer electrolyte as the lithium‐ion reservoir and α‐In₂Se₃as the channel material, the intercalated lithium concentration via a gate electric field is modulated. This manipulation drives a phase transition in α‐In₂Se₃from a ferroelectric semiconductor to a dirty metal and finally to a metal, accompanied by a structural transformation. Concurrently, with enhanced intercalation, the ferroelectric hysteresis window progressively narrows and eventually disappears, indicating the evolution from switchable to non‐switchable polarization. This study represents a promising platform for the artificial construction of correlated material systems, enabling a systematic investigation into the interaction of ferroelectricity and electronic conduction using ion intercalation. 

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.