LAUSR

There is considerable interest in van der Waals (vdW) materials as potential hosts for chiral skyrmionic spin textures. Of particular interest is the ferromagnetic, metallic compound Fe3GeTe2 (FGT), which has a comparatively high Curie temperature (150–220 K). Several recent studies have reported the observation of chiral Néel skyrmions in this compound, which is inconsistent with its presumed centrosymmetric structure. Here the observation of Néel type skyrmions in single crystals of FGT via Lorentz transmission electron microscopy (LTEM) is reported. It is shown from detailed X‐ray diffraction structure analysis that FGT lacks an inversion symmetry as a result of an asymmetric distribution of Fe vacancies. This vacancy‐induced breaking of the inversion symmetry of this compound is a surprising and novel observation and is a prerequisite for a Dzyaloshinskii–Moriya vector exchange interaction which accounts for the chiral Néel skyrmion phase. This phenomenon is likely to be common to many 2D vdW materials and suggests a path to the preparation of many such acentric compounds. Furthermore, it is found that the skyrmion size in FGT is strongly dependent on its thickness: the skyrmion size increases from ≈100 to ≈750 nm as the thickness of the lamella is increased from ≈90 nm to ≈2 µm. This extreme size tunability is a feature common to many low symmetry ferro‐ and ferri‐magnetic compounds.