Enhanced Magnetic Anisotropy in Strained V-Doped Janus WSSe Nanosheets: A First-Principles Study on Asymmetric d-p-d Hybridization with Implications for Spintronic Applications

High Resolution Image Download MS PowerPoint Slide Despite glimpses of promise, achieving long-range spin order at room temperature in magnetically doped two-dimensional (2D) semiconductors remains a major challenge. Two key strategies to enhance the Curie temperature ( T C ) in doped transition metal dichalcogenides (TMDs) are (1) optimizing hybridization for strong exchange coupling ( J ) and (2) enhancing local anisotropy for high magnetic anisotropy energy (MAE). In this study, we employ first-principles calculations and Monte Carlo simulations to investigate the electronic and magnetic properties of V-doped WS 2, WSe 2, and WSSe monolayers, with a focus on the orbital hybridization and strain tunability of WSSe. Our results reveal that WSSe inherits favorable properties from both base materials, WS 2 and WSe 2, making it a promising diluted magnetic semiconductor (DMS). While WSSe exhibits a slightly reduced d x 2 –y 2 –p x /p y – d x 2 –y 2 hybridization compared to WSe 2, it retains a substantial planar orbital overlap, which can be further enhanced under biaxial compressive strain. From WS 2, it inherits a significant d z 2 −p z 2 hybridization, which causes an increased MAE under compressive strain. Hence, this anisotropy in d-p-d hybridization can be a unique knob for controlling the magnetic properties of magnetically doped WSSe. Additionally, site- and orbital-resolved calculations confirm that MAE is primarily governed by neighboring W atoms, with the < d xy|Lz|dx 2 – y 2 > interaction playing a dominant role. The unique combination of asymmetric spin localization, exchange interactions, and strain-enhanced MAE establishes WSSe as a promising material for spintronic applications, offering a pathway toward next-generation magnetic TMD-based devices.