Pressure‐induced Sixfold Enhancement and Suppression of Topological Hall Effect in Two‐dimensional Chiral Magnet FeTa ₃ S ₆

ABSTRACT We report a pronounced and reversible pressure modulation of the hump‐like Hall anomaly assigned to the topological Hall effect (THE) in the two‐dimensional chiral magnet FeTa 3 S 6 . The additional Hall contribution reaches its maximum magnitude at 1.5 GPa, nearly six times larger than that at ambient pressure. This low‐pressure enhancement suggests that hydrostatic pressure modifies the structural conditions favorable for Dzyaloshinskii–Moriya interaction (DMI)‐related chiral magnetic textures and spin‐charge coupling. Upon further compression, the hump‐like Hall contribution is rapidly suppressed and disappears above ∼5 GPa, accompanied by a significant suppression of the anomalous Hall response. Raman spectroscopy, high‐pressure X‐ray diffraction, and density functional theory‐based structural relaxation indicate that pressure reduces the FeS6 octahedral distortion and weakens the local non‐centrosymmetric environment, which may suppress DMI‐related chiral magnetic textures. The Hall response recovers upon decompression, demonstrating the reversible tunability and structural robustness of FeTa 3 S 6 . Our findings establish hydrostatic pressure as a clean and reversible tuning parameter for probing the coupling among lattice distortion, chiral magnetic textures, and topological Hall transport in van der Waals magnets.