期刊
CHEMISTRY OF MATERIALS
卷 32, 期 2, 页码 795-804出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.9b04180
关键词
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资金
- Department of Defense (DoD) Air Force Office of Scientific Research (AFOSR) Young Investigator Program [FA9550-17-1-0170]
- National Science Foundation CAREER Award [1847370]
- U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences, Materials Science and Engineering Division
- U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences
- U.S. DOE, Iowa State University [DE-AC02-07CH11358]
- Ames Laboratory
- US Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division [DE-AC02-07CH11358]
- HPC@ISU equipment at Iowa State University
- NSF under MRI [CNS 1726447]
- National Science Foundation Graduate Research Fellowship Program [DGE 1744592]
- Herbert L. Stiles Faculty Fellowship
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1847370] Funding Source: National Science Foundation
Si-nanosheets (Si-NSs) have recently attracted considerable attention due to their potential as next-generation materials for electronic, optoelectronic, spintronic, and catalytic applications. Even though monolayer Si-NSs were first synthesized over 150 years ago via topotactic deintercalation of CaSi2, there is a lack of consensus within the literature regarding the structure and optical properties of this material. Herein, we provide conclusive evidence of the structural and chemical properties of Si-NSs produced by the deintercalation of CaSi2 with cold (similar to-30 degrees C) aqueous HCl and characterize their optical properties. We use a wide range of techniques, including XRD, FTIR, Raman, solid-state NMR, SEM, TEM, EDS, XPS, diffuse reflectance absorbance, steady-state photoluminescence, time-resolved photoluminescence, and thermal decomposition; when they are combined together, these techniques enable unique insight into the structural and optical properties of the Si-NSs. Additionally, we support the experimental findings with density functional theory (DFT) calculations to simulate FTIR, Raman, solid-state NMR, interband electronic transitions, and band structures. We determined that the Si-NSs consist of buckled Si monolayers that are primarily monohydride terminated. We characterize the nanosheet optical properties, finding they have a band gap of similar to 2.5 eV with direct-like behavior and an estimated quantum yield of similar to 9%. Given the technological importance of Si, these results are encouraging for a variety of optoelectronic technologies, such as phosphors, light-emitting diodes, and CMOS-compatible photonics. Our results provide critical structural and optical properties to help guide the research community in integrating Si-NSs into optoelectronic and quantum devices.
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