Symmetry-Engineering-Induced In-Plane Polarization Enhancement in Ta₂NiS₅/CrOCl van der Waals Heterostructure

Van der Waals (vdW) interfaces can be formed via layer stacking regardless of the lattice constant or symmetry of the individual building blocks. Herein, we constructed a vdW interface of layered Ta₂NiS₅ and CrOCl, which exhibited remarkably enhanced in-plane anisotropy via polarized Raman spectroscopy and electrical transport measurements. Compared with pristine Ta₂NiS₅, the anisotropy ratio of the Raman intensities for the B_2g, ²A_g, and ³A_g modes increased in the heterostructure. More importantly, the anisotropy ratios of conductivity and mobility in the heterostructure increased by one order of magnitude. Specifically speaking, the conductivity ratio changed from ~2.1 (Ta₂NiS₅) to ~15 (Ta₂NiS₅/CrOCl), while the mobility ratio changed from ~2.7 (Ta₂NiS₅) to ~32 (Ta₂NiS₅/CrOCl). Such prominent enhancement may be attributed to the symmetry reduction caused by lattice mismatch at the heterostructure interface and the introduction of strain into the Ta₂NiS₅. Our research provides a new perspective for enhancing artificial anisotropy physics and offers feasible guidance for future functionalized electronic devices.