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Unusually high exciton binding energies (BEs), as much as ∼1 eV in monolayer transition-metal dichalcogenides, provide opportunities for exploring exotic and stable excitonic many-body effects. These include many-body neutral excitons, trions, biexcitons, and defect-induced excitons at room temperature, rarely realized in bulk materials. Nevertheless, the defect-induced trions correlated with charge screening have never been observed, and the corresponding BEs remain unknown. Here we report defect-induced A-trions and B-trions in monolayer tungsten disulfide (WS2) via carrier screening engineering with photogenerated carrier modulation, external doping, and substrate scattering. Defect-induced trions strongly couple with inherent SiO2 hole traps under high photocarrier densities and become more prominent in rhenium-doped WS2. The absence of defect-induced trion peaks was confirmed using a trap-free hexagonal boron nitride substrate, regardless of power density. Moreover, many-body excitonic charge states and their BEs were compared via carrier screening engineering at room temperature. The highest BE was observed in the defect-induced A-trion state (∼214 meV), comparably higher than the trion (209 meV) and neutral exciton (174 meV), and further tuned by external photoinduced carrier density control. This investigation allows us to demonstrate defect-induced trion BE localization via spatial BE mapping in the monolayer WS2 midflake regions distinctive from the flake edges.

Rotationally aligned, two-dimensional (2D), transition-metal dichalcogenides (TMDs) exhibit unique electronic, optical, and optoelectronic properties compared to random stacking. Rotationally aligned graphene stacking was demonstrated previously for numerous exotic phenomena, such as superconductivity, resonant tunneling, and moire pattern. However, rotationally aligned drytransfer techniques of TMDs, have yet to be demonstrated. Here, we show a simple method of selective cutting of a few-layer tungsten diselenide (WSe2) flake and rotationally aligning it by using dry-transfer stacking. The dry transfer techniques used for this study were adapted to maintain low sample contamination, a high-quality interface, a low number of defects. A combination of viscoelastic and thermoelastic materials was used for the TMD pickup and release to facilitate the rotationally aligned stacking. Aligned WSe2 stacks were characterized by Raman and photoluminescence spectroscopy to evaluate the integrity of the fabricated stack. This study highlights the possibility of using a rotationally aligned, artificial stacking method for exfoliated TMD materials for future electronic and optoelectronic applications.

A dimensionally confined dielectric constant and reduced dielectric screening lead to two-dimensional transition-metal dichalcogenides (TMDs). The confined dielectric constant triggers a strong Coulomb interaction and high exciton binding energies between TMD heterostructures. Here we show a highly efficient interlayer charged exciton or trion formation and its generation sites are present in materials at room temperature. Two different transition metals (Mo, W) and chalcogenide (S, Se) elements were investigated in two different heterostructure combinations (MoS2—WS2 and MoSe2—WS2). Room temperature photoluminescence measurements demonstrate a highly efficient trion formation between and close to the heterostructure interfaces. This study highlights an effective band alignment, strong photoexciting Coulomb interaction, and formation of interlayer trions with different recombination energies. This investigation suggests the possibility of utilizing interlayer trions in promising optoelectronic devices in the future.