Proton/Oxygen Dual‐Ion Gated Control of Skyrmion Nucleation via Tuning Orbital Asymmetry

The pure voltage control of skyrmions represents a promising approach for developing skyrmion devices with low power consumption and high stability. However, existing methods still face long‐standing challenges in terms of reliance on an assisted magnetic field and fast control of small‐sized skyrmions at low voltages. This work proposes an ionic‐liquid (IL) gating strategy based on the electric‐field induced magnetoionic effect (EIME). The applied electric field activates H + /O 2− migration in the Pt/Co/Al 2 O 3 multilayer at a low voltage (±4 V), enabling the pure‐voltage‐controlled nucleation and annihilation of skyrmions in a reversible and non‐volatile way. Microscopically, the electric‐field‐driven migration of dual ions modifies both the interface and bulk attributes such as the Co‐O hybridization and orbital asymmetry of Co, thereby regulating both the Dzyaloshinskii‐Moriya interaction (DMI) and Heisenberg interactions through changes in orbital and spin moments. These findings clarify the indirect ion‐skyrmion coupling mechanism at the electronic level and highlight a promising pathway for ion‐governed skyrmion devices.