Hidden Valley Polarization, Piezoelectricity, and Dzyaloshinskii–Moriya Interactions of Janus Vanadium Dichalcogenides

Due to the lack of inversion symmetry and the discovery of room-temperature ferromagnetism, two-dimensional semiconducting vanadium-based van der Waals transition-metal dichalcogenides (V-TMDs) are drawing attention for their possible application in spintronics and valleytronics. Here, we show the functional properties enriched by the broken inversion, out-of-plane mirror, and time-reversal symmetries of Janus H–VXY TMDs (X, Y = S, Se, Te). By first-principles calculations, we reveal the intrinsic xy easy-plane magnetism of the Janus vanadium-based TMD monolayers and systematically study their hidden valley polarization and giant magneto band structure. Their strong nearest-neighbor exchange strengths lead to near-room-temperature magnetic phase transitions. The Janus H–VXY system also exhibits piezoelectricity with nonzero e₃₁ and e₂₁. Interestingly, it is found that the right-handed Dzyaloshinskii–Moriya interaction has nonzero in-plane components in our Janus system, with fluctuating magnitudes determined by competence between relaxed bond-angle and atomic index of ligands.