Journal
NANO LETTERS
Volume 14, Issue 2, Pages 442-449Publisher
AMER CHEMICAL SOC
DOI: 10.1021/nl4032296
Keywords
Monolayer molybdenum disulfide (MoS2); ternary alloy; Se doping; dopant distribution; ADF imaging; band gap engineering
Categories
Funding
- Army Research Office MURI [W911NF-11-1-0362]
- FAME Center, One of six centers of STARnet, a Semiconductor Research Corporation program
- MARCO
- DARPA
- U.S. Office of Naval Research MURI [N000014-09-1-1066]
- Welch Foundation [C-1716]
- NSF [DMR-0928297]
- National Research Foundation Singapore under NRF RF Award [NRF-RF2013-08]
- Nanoelectronics Research Corporation [S201006]
- Materials Simulation Center of the Materials Research Institute
- Research Computing and Cyberinfrastructure unit of Information Technology Services
- Penn-State Center for Nanoscale Science
- Wigner Fellowship through the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory (ORNL)
- U.S. Department of Energy (DOE), Basic Energy Sciences, Materials Sciences and Engineering Division
- U.S. DOE [DE-FG02-09ER46554]
- ORNL's Center for Nanophase Materials Sciences (CNMS)
- Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. DOE
- JST-Japan under Japanese regional Innovation Strategy Program by the Excellence
- Penn State Center for Nanoscale Science [DMR-0820404]
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Ternary two-dimensional dichalcogenide alloys exhibit compositionally modulated electronic structure, and hence, control of dopant concentration within each individual layer of these compounds provides a powerful tool to efficiently modify their physical and chemical properties. The main challenge arises when quantifying and locating the dopant atoms within each layer in order to better understand and fine-tune the desired properties. Here we report the synthesis of molybdenum disulfide substitutionally doped with a broad range of selenium concentrations, resulting in over 10% optical band gap modulations in atomic layers. Chemical analysis using Z-contrast imaging provides direct maps of the dopant atom distribution in individual MoS2 layers and hence a measure of the local optical band gaps. Furthermore, in a bilayer structure, the dopant distribution is imaged layer-by-layer. This. work demonstrates that each layer in the bilayer system contains similar local Se concentrations, randomly distributed, providing new insights into the growth mechanism and alloying behavior in two-dimensional dichalcogenide atomic layers. The results show that growth of uniform, ternary, two-dimensional dichalcogenide alloy films with tunable electronic properties is feasible.
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