Transition Metal Dichalcogenides: Making Atomic-Level Magnetism Tunable with Light at Room Temperature

The capacity to manipulate magnetization in 2D dilute magnetic semiconductors (2D-DMSs) using light, specifically in magnetically doped transition metal dichalcogenide (TMD) monolayers (M-doped TX2, where M = V, Fe, and Cr; T = W, Mo; X = S, Se, and Te), may lead to innovative applications in spintronics, spin-caloritronics, valleytronics, and quantum computation. This Perspective paper explores the mediation of magnetization by light under ambient conditions in 2D-TMD DMSs and heterostructures. By combining magneto-LC resonance (MLCR) experiments with density functional theory (DFT) calculations, we show that the magnetization can be enhanced using light in V-doped TMD monolayers (e.g., V-WS2, V-WSe2). This phenomenon is attributed to excess holes in the conduction and valence bands, and carriers trapped in magnetic doping states, mediating the magnetization of the semiconducting layer. In 2D-TMD heterostructures (VSe2/WS2, VSe2/MoS2), the significance of proximity, charge-transfer, and confinement effects in amplifying light-mediated magnetism is demonstrated. We attributed this to photon absorption at the TMD layer that generates electron-hole pairs mediating the magnetization of the heterostructure. These findings will encourage further research in the field of 2D magnetism and establish a novel design of 2D-TMDs and heterostructures with optically tunable magnetic functionalities, paving the way for next-generation magneto-optic nanodevices. Both experimentally and theoretically it is demonstrated that the magnetization of a 2D dilute magnetic semiconductor based on a V-doped transition metal dichalcogenide (TMD) monolayer or a 2D-TMD heterostructure composed of metallic (magnetic) and semiconducting (non-magnetic) TMD layers can be optically tuned. This establishes a novel direction for designing 2D-TMDs and heterostructures with optically tunable magnetic functionalities for next-generation nanodevices.image