Substitutionally doped transition metal dichalcogenides (TMDs) are essential for advancing TMD‐based field effect transistors, sensors, and quantum photonic devices. However, the impact of local dopant concentrations and dopant–dopant interactions on charge doping and defect formation within TMDs remains underexplored. Here, a breakthrough understanding of the influence of rhenium (Re) concentration is presented on charge doping and defect formation in MoS2monolayers grown by metal–organic chemical vapor deposition (MOCVD). It is shown that Re‐MoS2films exhibit reduced sulfur‐site defects, consistent with prior reports. However, as the Re concentration approaches ⪆2 atom%, significant clustering of Re in the MoS2is observed. Ab Initio calculations indicate that the transition from isolated Re atoms to Re clusters increases the ionization energy of Re dopants, thereby reducing Re‐doping efficacy. Using photoluminescence (PL) spectroscopy, it is shown that Re dopant clustering creates defect states that trap photogenerated excitons within the MoS2lattice, resulting in broad sub‐gap emission. These results provide critical insights into how the local concentration of metal dopants influences carrier density, defect formation, and exciton recombination in TMDs, offering a novel framework for designing future TMD‐based devices with improved electronic and photonic properties.
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Evolution of defect formation during atomically precise desulfurization of monolayer MoS2
Abstract Structural symmetry-breaking is a key strategy to modify the physical and chemical properties of two-dimensional transition metal dichalcogenides. However, little is known about defect formation during this process. Here, with atomic-scale microscopy, we investigate the evolution of defect formation in monolayer MoS 2 exposed indirectly to hydrogen plasma. At the beginning of the treatment only top-layer sulfur atoms are removed, while vacancies and the molybdenum atomic layer are maintained. As processing continues, hexagonal-shaped nanocracks are generated along the zigzag edge during relaxation of defect-induced strain. As defect density increases, both photoluminescence and conductivity of MoS 2 gradually decreases. Furthermore, MoS 2 showed increased friction by 50% due to defect-induced contact stiffness. Our study reveals the details of defect formation during the desulfurization of MoS 2 and helps to design the symmetry-breaking transition metal dichalcogenides, which is of relevance for applications including photocatalyst for water splitting, and Janus heterostructures.
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- Award ID(s):
- 1720633
- PAR ID:
- 10330203
- Date Published:
- Journal Name:
- Communications Materials
- Volume:
- 2
- Issue:
- 1
- ISSN:
- 2662-4443
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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