Silicene, Siloxene, or Silicane? Revealing the Structure and Optical Properties of Silicon Nanosheets Derived from Calcium Disilicide
datasetposted on 03.12.2019 by Bradley J. Ryan, Michael P. Hanrahan, Yujie Wang, Utkarsh Ramesh, Charles K. A. Nyamekye, Rainie D. Nelson, Zhaoyu Liu, Chuankun Huang, Bevan Whitehead, Jigang Wang, Luke T. Roling, Emily A. Smith, Aaron J. Rossini, Matthew G. Panthani
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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 (∼−30 °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 ∼2.5 eV with direct-like behavior and an estimated quantum yield of ∼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.