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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.
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MoS 2 pixel arrays for real-time photoluminescence imaging of redox molecules
Measuring the behavior of redox-active molecules in space and time is crucial for understanding chemical and biological systems and for developing new technologies. Optical schemes are noninvasive and scalable, but usually have a slow response compared to electrical detection methods. Furthermore, many fluorescent molecules for redox detection degrade in brightness over long exposure times. Here, we show that the photoluminescence of “pixel” arrays of monolayer MoS 2 can image spatial and temporal changes in redox molecule concentration. Because of the strong dependence of MoS 2 photoluminescence on doping, changes in the local chemical potential substantially modulate the photoluminescence of MoS 2 , with a sensitivity of 0.9 mV / Hz on a 5 μm × 5 μm pixel, corresponding to better than parts-per-hundred changes in redox molecule concentration down to nanomolar concentrations at 100-ms frame rates. This provides a new strategy for visualizing chemical reactions and biomolecules with a two-dimensional material screen.
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- Award ID(s):
- 1719875
- PAR ID:
- 10146299
- Date Published:
- Journal Name:
- Science Advances
- Volume:
- 5
- Issue:
- 11
- ISSN:
- 2375-2548
- Page Range / eLocation ID:
- eaat9476
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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We report a comprehensive study on the effects of rhenium doping on optical properties and photocarrier dynamics of MoS 2 monolayer, few-layer, and bulk samples. Monolayer and few-layer samples of Re-doped (0.6%) and undoped MoS 2 were fabricated by mechanical exfoliation, and were studied by Raman spectroscopy, optical absorption, photoluminescence, and time-resolved differential reflection measurements. Similar Raman, absorption, and photoluminescence spectra were obtained from doped and undoped samples, indicating that the Re doping at this level does not significantly alter the lattice and electronic structures. Red-shift and broadening of the two phonon Raman modes were observed, showing the lattice strain and carrier doping induced by Re. The photoluminescence yield of the doped monolayer is about 15 times lower than that of the undoped sample, while the photocarrier lifetime is about 20 times shorter in the doped monolayer. Both observations can be attributed to diffusion-limited Auger nonradiative recombination of photocarriers at Re dopants. These results provide useful information for developing a doping strategy of MoS 2 for optoelectronic applications.more » « less
- Free Publicly Accessible Full Text
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Accepted Manuscript
- Journal Article:
- https://doi.org/10.1126/sciadv.aat9476
