Controllable Skyrmionic Phase Transition between Néel Skyrmions and Bloch Skyrmionic Bubbles in van der Waals Ferromagnet Fe 3‐δ GeTe 2

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The van der Waals (vdW) ferromagnet Fe 3‐δ GeTe 2 has garnered significant research interest as a platform for skyrmionic spin configurations, that is, skyrmions and skyrmionic bubbles. However, despite extensive efforts, the origin of the Dzyaloshinskii–Moriya interaction (DMI) in Fe 3‐δ GeTe 2 remains elusive, making it challenging to acquire these skyrmionic phases in a controlled manner. In this study, it is demonstrated that the Fe content in Fe 3‐δ GeTe 2 has a profound effect on the crystal structure, DMI, and skyrmionic phase. For the first time, a marked increase in Fe atom displacement with decreasing Fe content is observed, transforming the original centrosymmetric crystal structure into a non‐centrosymmetric symmetry, leading to a considerable DMI. Additionally, by varying the Fe content and sample thickness, a controllable transition between Néel‐type skyrmions and Bloch‐type skyrmionic bubbles is achieved, governed by a delicate interplay between dipole–dipole interaction and the DMI. The findings offer novel insights into the variable skyrmionic phases in Fe 3‐δ GeTe 2 and provide the impetus for developing vdW ferromagnet‐based spintronic devices.