Dilute magnetic semiconductors (DMS), achieved through substitutional doping of spin-polarized transition metals into semiconducting systems, enable experimental modulation of spin dynamics in ways that hold great promise for novel magneto-electric or magneto-optical devices, especially for two-dimensional (2D) systems such as transition metal dichalcogenides that accentuate interactions and activate valley degrees of freedom. Practical applications of 2D magnetism will likely require room-temperature operation, air stability, and (for magnetic semiconductors) the ability to achieve optimal doping levels without dopant aggregation. Here, room-temperature ferromagnetic order obtained in semiconducting vanadium-doped tungsten disulfide monolayers produced by a reliable single-step film sulfidation method across an exceptionally wide range of vanadium concentrations, up to 12 at% with minimal dopant aggregation, is described. These monolayers develop p-type transport as a function of vanadium incorporation and rapidly reach ambipolarity. Ferromagnetism peaks at an intermediate vanadium concentration of˜2 at% and decreases for higher concentrations, which is consistent with quenching due to orbital hybridization at closer vanadium-vanadium spacings, as supported by transmission electron microscopy, magnetometry, and first-principles calculations. Room-temperature 2D-DMS provide a new component to expand the functional scope of van der Waals heterostructures and bring semiconducting magnetic 2D heterostructures into the realm of practical application.

Doping lies at the heart of modern semiconductor technologies. Therefore, for two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs), the significance of controlled doping is no exception. Recent studies have indicated that, by substitutionally doping 2D TMDs with a judicious selection of dopants, their electrical, optical, magnetic, and catalytic properties can be effectively tuned, endowing them with great potential for various practical applications. Herein, and inspired by the sol–gel process, we report a liquid-phase precursor-assisted approach for in situ substitutional doping of monolayered TMDs and their in-plane heterostructures with tunable doping concentration. This highly reproducible route is based on the high-temperature chalcogenation of spin-coated aqueous solutions containing host and dopant precursors. The precursors are mixed homogeneously at the atomic level in the liquid phase prior to the synthesis process, thus allowing for an improved doping uniformity and controllability. We further demonstrate the incorporation of various transition metal atoms, such as iron (Fe), rhenium (Re), and vanadium (V), into the lattice of TMD monolayers to form Fe-doped WS2, Re-doped MoS2, and more complex material systems such as V-doped in-plane W x Mo1–x S2–Mo x W1–x S2 heterostructures, among others. We envisage that our developed approach is universal and could be extended to incorporate a variety of other elements into 2D TMDs and create in-plane heterointerfaces in a single step, which may enable applications such as electronics and spintronics at the 2D limit.

The outstanding optoelectronic and valleytronic properties of transition metal dichalcogenides (TMDs) have triggered intense research efforts by the scientific community. An alternative to induce long‐range ferromagnetism (FM) in TMDs is by introducing magnetic dopants to form a dilute magnetic semiconductor. Enhancing ferromagnetism in these semiconductors not only represents a key step toward modern TMD‐based spintronics, but also enables exploration of new and exciting dimensionality‐driven magnetic phenomena. To this end, tunable ferromagnetism at room temperature and a thermally induced spin flip (TISF) in monolayers of V‐doped WSe2 are shown. As vanadium concentration increases, the saturation magnetization increases, which is optimal at ≈4 at% vanadium; the highest doping level ever achieved for V‐doped WSe2 monolayers. The TISF occurs at ≈175 K and becomes more pronounced upon increasing the temperature toward room temperature. The TISF can be manipulated by changing the vanadium concentration. The TISF is attributed to the magnetic‐field‐ and temperature‐dependent flipping of the nearest W‐site magnetic moments that are antiferromagnetically coupled to the V magnetic moments in the ground state. This is fully supported by a recent spin‐polarized density functional theory study. The findings pave the way for the development of novel spintronic and valleytronic nanodevices and stimulate further research.

carried out to explore Fano resonances that arise from the coupling between surface plasmons (SPs) and excitons in quantum dots (QDs) or dye molecules. [2,[6][7][8][9][10][11] However, the lack of efficient ways to actively tune the excitonic properties of QDs and dye molecules near plasmonic nanostructures makes the development of active devices based on hybrid plasmon-QD/ dye systems challenging. Recently, the interaction between plasmonic nanostructures and emerging 2D semiconductors, including monolayer transition metal dichalcogenides (TMDCs), has attracted the attention of various researchers. [12][13][14] monolayer TMDCs possess high carrier mobility, direct bandgap, and strong excitonic and mechanical properties. Combining these outstanding properties with plasmonic nanostructures, able to confine light at the subwavelength scale and generate energetic hot electrons, holds the promise to enhance the performance of monolayer TMDC-based optoelectronic components and boost the development of miniaturized Strong spatial confinement and highly reduced dielectric screening provide monolayer transition metal dichalcogenides with strong many-body effects, thereby possessing optically forbidden excitonic states (i.e., dark excitons) at room temperature. Herein, the interaction of surface plasmons with dark excitons in hybrid systems consisting of stacked gold nanotriangles and monolayer WS 2 is explored. A narrow Fano resonance is observed when the hybrid system is surrounded by water, and the narrowing of the spectral Fano linewidth is attributed to the plasmon-enhanced decay of dark K-K excitons. These results reveal that dark excitons in monolayer WS 2 can strongly modify Fano resonances in hybrid plasmon-exciton systems and can be harnessed for novel optical sensors and active nanophotonic devices.

Atomically thin transition metal dichalcogenide (TMD) semiconductors hold enormous potential for modern optoelectronic devices and quantum computing applications. By inducing long-range ferromagnetism (FM) in these semiconductors through the introduction of small amounts of a magnetic dopant, it is possible to extend their potential in emerging spintronic applications. Here, we demonstrate light-mediated, room temperature (RT) FM, in V-doped WS 2 (V-WS 2 ) monolayers. We probe this effect using the principle of magnetic LC resonance, which employs a soft ferromagnetic Co-based microwire coil driven near its resonance in the radio frequency (RF) regime. The combination of LC resonance with an extraordinary giant magneto-impedance effect, renders the coil highly sensitive to changes in the magnetic flux through its core. We then place the V-WS 2 monolayer at the core of the coil where it is excited with a laser while its change in magnetic permeability is measured. Notably, the magnetic permeability of the monolayer is found to depend on the laser intensity, thus confirming light control of RT magnetism in this two-dimensional (2D) material. Guided by density functional calculations, we attribute this phenomenon to the presence of excess holes in the conduction and valence bands, as well as carriers trapped in the magnetic doping states, which in turn mediates the magnetization of the V-WS 2 monolayer. These findings provide a unique route to exploit light-controlled ferromagnetism in low powered 2D spintronic devices capable of operating at RT.