Unusual Dzyaloshinskii‐Moriya Interaction in Graphene/Fe₃GeTe₂ Van der Waals Heterostructure

Abstract

Dzyaloshinskii–Moriya interaction (DMI) is shown to induce a topologically protected chiral spin texture in magnetic/nonmagnetic heterostructures. In the context of van der Waals spintronic devices, graphene emerges as an excellent candidate material. However, due to its negligible spin‐orbit interaction, inducing DMI to stabilize topological spins when coupled to 3d‐ferromagnets remains challenging. Here, it is demonstrated that, despite these challenges, a sizeable Rashba‐type spin splitting followed by significant DMI is induced in graphene/Fe3GeTe2. This is made possible due to an interfacial electric field driven by charge asymmetry together with the broken inversion symmetry of the heterostructure. These findings reveal that the enhanced DMI energy parameter, resulting from a large effective electron mass in Fe3GeTe2, remarkably contributes to stabilizing non‐collinear spins below the Curie temperature, overcoming the magnetic anisotropy energy. These results are supported by the topological Hall effect, which coexists with the non‐trivial breakdown of Fermi liquid behavior, confirming the interplay between spins and non‐trivial topology. This work paves the way toward the design and control of interface‐driven skyrmion‐based devices.