Tailoring Dzyaloshinskii-Moriya interaction in a transition metal dichalcogenide by dual-intercalation

Dzyaloshinskii-Moriya interaction (DMI) is vital to form various chiral spin textures, novel behaviors of magnons and permits their potential applications in energy-efficient spintronic devices. Here, we realize a sizable bulk DMI in a transition metal dichalcogenide (TMD) 2H-TaS₂ by intercalating Fe atoms, which form the chiral supercells with broken spatial inversion symmetry and also act as the source of magnetic orderings. Using a newly developed protonic gate technology, gate-controlled protons intercalation could further change the carrier density and intensely tune DMI via the Ruderman-Kittel-Kasuya-Yosida mechanism. The resultant giant topological Hall resistivity [Formula: see text] of [Formula: see text] at [Formula: see text] (about [Formula: see text] larger than the zero-bias value) is larger than most known chiral magnets. Theoretical analysis indicates that such a large topological Hall effect originates from the two-dimensional Bloch-type chiral spin textures stabilized by DMI, while the large anomalous Hall effect comes from the gapped Dirac nodal lines by spin-orbit interaction. Dual-intercalation in 2H-TaS₂ provides a model system to reveal the nature of DMI in the large family of TMDs and a promising way of gate tuning of DMI, which further enables an electrical control of the chiral spin textures and related electromagnetic phenomena.