Magneto‐Ionic Engineering of Antiferromagnetically RKKY‐Coupled Multilayers

Voltage‐driven ion motion offers a powerful means to modulate magnetism and spin phenomena in solids, a process known as magneto‐ionics, which holds great promise for developing energy‐efficient next‐generation micro‐ and nano‐electronic devices. Synthetic antiferromagnets (SAFs), consisting of two ferromagnetic layers coupled antiferromagnetically via a thin non‐magnetic spacer, offer advantages such as enhanced thermal stability, robustness against external magnetic fields, and reduced magnetostatic interactions in magnetic tunnel junctions. Despite its technological potential, magneto‐ionic control of antiferromagnetic coupling in multilayers (MLs) has only recently been explored and remains poorly understood, particularly in systems free of platinum‐group metals. In this work, room‐temperature voltage control of Ruderman–Kittel–Kasuya–Yosida (RKKY) interactions in Co/Ni‐based SAFs is achieved. Transitions between ferrimagnetic (uncompensated) and antiferromagnetic (fully compensated) states is observed, as well as significant modulation of the RKKY bias field offset, emergence of additional switching events, and formation of skyrmion‐like or pinned domain bubbles under relatively low gating voltages. These phenomena are attributed to voltage‐driven oxygen migration in the MLs, as confirmed through microscopic and spectroscopic analyses. This study underscores the potential of voltage‐triggered ion migration as a versatile tool for post‐synthesis tuning of magnetic multilayers, with potential applications in magnetic‐field sensing, energy‐efficient memories and spintronics.