Identifying Defect-Induced Trion in Monolayer WS₂ <i>via</i> Carrier Screening Engineering.

Abstract

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) <i>via</i> 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 <i>via</i> 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 <i>via</i> spatial BE mapping in the monolayer WS₂ midflake regions distinctive from the flake edges.