Antiferromagnetic Single Crystalline VTe₂ with Double Zigzag Chain-Like Modulation

Recently, two-dimensional (2D) ferromagnetic materials have rapidly garnered much interest for the future spintronic and quantum computing devices, where they may serve the implementation of spin-transfer torque memory. In addition, the multiple polymorphic phases in a single material can lead to the exotic physical properties, stimulating to investigate discovery of new materials or modification of well-known materials. Here, we demonstrate that highly single crystalline VTe₂ with double zigzag chain structure has antiferromagnetic ordering, verified by temperature dependent Raman spectra and theoretical calculations. The lattice parameters estimated by in-depth diffraction patterns analyses reveal monoclinic structure unlike previous reported hexagonal structure. Interestingly, the Raman peaks related to phonon vibration modes of VTe₂ are saturated, while two Raman peaks newly emerge at very low temperatures, originating from antiferromagnetic ordering. By the bulk density functional theory calculation, we find that distorted zigzag structure is the most stable structure in considered VTe₂ atomic configuration and stronger in-plane magnetic interaction than that across the van der Waals gap. Our findings not only provide insight into further 2D vanadium-based chalcogenides, but also pave the way toward practical incorporation of 2D ferromagnetic materials.