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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. 

Abstract Realizing stimulated emission from defects in 2D‐layered semiconductors has the potential to enhance the sensitivity of characterizing their defects. However, stimulated emission from defects in layered materials presents a different set of challenges in carrier lifetime and energy level design and is not achieved so far. Here, photoluminescence (PL) spectroscopy, Raman spectroscopy, and first‐principles theory are combined to reveal an anomalous PL intensity–temperature relation and strong polarization effects at a defect emission peak in annealed multilayer MoS₂, suggesting defect‐based stimulated emission. The emergence of stimulated emission behavior is also controllable (by temperature) and reversible. The observed stimulated emission behavior is supported by a three‐level system involving two defect levels from chalcogen vacancies and a pump level from the conduction band edge. First‐principles calculations show that the special indirect gap that enables stimulated emission is not native to pristine bulk MoS₂and only emerges under thermal strain.