Low‐Defect‐Density Monolayer MoS₂ Wafer by Oxygen‐Assisted Growth‐Repair Strategy

Atomic chalcogen vacancy is the most commonly observed defect category in two dimensional (2D) transition-metal dichalcogenides, which can be detrimental to the intrinsic properties and device performance. Here a low-defect density, high-uniform, wafer-scale single crystal epitaxial technology by in situ oxygen-incorporated "growth-repair" strategy is reported. For the first time, the oxygen-repairing efficiency on MoS₂ monolayers at atomic scale is quantitatively evaluated. The sulfur defect density is greatly reduced from (2.71 ± 0.65) × 10¹³ down to (4.28 ± 0.27) × 10¹² cm^-2, which is one order of magnitude lower than reported as-grown MoS₂. Such prominent defect deduction is owing to the kinetically more favorable configuration of oxygen substitution and an increase in sulfur vacancy formation energy around oxygen-incorporated sites by the first-principle calculations. Furthermore, the sulfur vacancies induced donor defect states is largely eliminated confirmed by quenched defect-related emission. The devices exhibit improved carrier mobility by more than three times up to 65.2 cm² V^-1 s^-1 and lower Schottky barrier height reduced by half (less than 20 meV), originating from the suppressed Fermi-level pinning effect from disorder-induced gap state. The work provides an effective route toward engineering the intrinsic defect density and electronic states through modulating synthesis kinetics of 2D materials.