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 $${\rho }_{{xy}}^{T}$$ ρ x y T of $$1.41{\mathrm{\mu}} \Omega \cdot {{\mathrm{cm}}}$$ 1.41 μ Ω ⋅ cm at $${V}_{g}=-5.2{\mathrm{V}}$$ V g = − 5.2 V (about $$424 \%$$ 424 % 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.