J. Semicond. > 2023, Volume 44 > Issue 4 > 041101, doi: 10.1088/1674-4926/44/4/041101
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REVIEWS

Two-dimensional silicon nanomaterials for optoelectronics

Xuebiao Deng, Huai Chen and Zhenyu Yang

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 Corresponding author: Zhenyu Yang, yangzhy63@mail.sysu.edu.cn

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Abstract: Silicon nanomaterials have been of immense interest in the last few decades due to their remarkable optoelectronic responses, elemental abundance, and higher biocompatibility. Two-dimensional silicon is one of the new allotropes of silicon and has many compelling properties such as quantum-confined photoluminescence, high charge carrier mobilities, anisotropic electronic and magnetic response, and non-linear optical properties. This review summarizes the recent advances in the synthesis of two-dimensional silicon nanomaterials with a range of structures (silicene, silicane, and multilayered silicon), surface ligand engineering, and corresponding optoelectronic applications.

Key words: two-dimensionality, silicon, nanomaterials, synthesis, surface engineering, optoelectronics



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Fig. 1.  (Color online) Schematic illustration of three types of 2D silicon nanomaterials. Silicene refers to the monolayered hexagonal lattice with sp2-sp3 hybridized Si atoms; silicane refers to the monolayered hexagonal lattice with sp3 hybridized Si atoms fully or partially passivated by ligands such as hydride, hydroxyl, alkyl groups; multilayered silicon nanosheet refers to the diamond-structured silicon with a thickness of a few atomic Si layers.

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Fig. 2.  (Color online) Preparation of 2D silicon nanomaterials. (a, b) Schematic illustration of two general synthetic approaches: epitaxial growth and chemical exfoliation. (c) STM image of a single-layered silicene island on Ag(111). (d) High-resolution STM image of monolayer silicene terrace showing the $\sqrt{3}$ × $\sqrt{3}$ honeycomb superstructure. Reprinted with permission from Ref. [29]. Copyright 2012 by American Chemical Society. (e) Scanning electron microscopic (SEM) images of freestanding MSNs prepared using the epitaxial growth method. Reprinted with permission from Ref. [30]. Copyright 2014 by American Chemical Society. (f) SEM image of layered silicanes obtained from the chemical exfoliation of CaSi2. Reprinted with permission from Ref. [27]. Copyright 2020 by American Chemical Society.

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Fig. 3.  (Color online) Schematic illustration of some recently reported surface modification approaches of 2DSis. R = alkyl/aryl group; Ph = phenyl; Bn = benzyl.

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Fig. 4.  (Color online) Material properties of surface-modified 2DSis. (a) Structural models of regularly stacked (C10-Sin). (b) AFM phase image of decylamine-functionalized silicane (C10-Sin) on a highly oriented pyrolytic graphite plate. (c) X-ray diffraction (XRD) pattern of C10-Sin with strong signals corresponding to the layered structure of silicane. (d) PL spectrum of the amine-passivated silicane. Reprinted with permission from Ref. [44]. Copyright 2010 by American Chemical Society. (e) Hybrid materials containing silicanes and polymers shows enhanced materials stability and PL property under continuous UV irradiation. Reprinted with permission from Ref. [77]. Copyright 2016 by Wiley-VCH.

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Fig. 5.  Proposed mechanisms of the hydrosilylation reaction on 2DSis[86, 93].

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Fig. 6.  (Color online) Surface modification of silicanes using single-step approaches. (a) Side view and (b) top view of the model structure of silicane partially passivated by hydride and phenyl groups (Si6H4Ph2). (c) PL spectra of Si6H4Ph2 thin film and solution (solvent:1,4-dioxane, excitation wavelength: 350 nm). Inset: blue emitting Si6H4Ph2 dispersed in 1,4-dioxane under 365 nm UV irradiation. Reprinted with permission from Ref. [94]. Copyright 2010 by American Chemical Society. (d) Hydride- and benzyl-passivated silicane directly made by the solvent-assisted chemical exfoliation of CaSi2 (e) Diffuse reflectance spectra of hydride-passivated (black) and benzyl-passivated 2DSis (red). Inset: Tauc plots of both 2DSi samples. Reprinted with permission from Ref. [95]. Copyright 2019 by American Chemical Society.

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Fig. 7.  (Color online) Electronic structures of pristine and surface-modified silicene. (a) Monte Carlo simulation results of temperature-dependent drift velocity behaviors of monolayer silicene (with or without out-of-plane acoustic (ZA)): 50 K (square), 100 K (triangle), 200 K (diamond), and 300 K (circle). Reprinted with permission from Ref. [103]. Copyright 2013 by American Physical Society. (b–g) The partial density of states of various types of surface-modified silicene: (b) pristine (i.e., “naked”) silicene, (c) hydride-terminated silicene, (d) hydrosilylated silicene, (e) phenylated silicene, (f) alkoxylated silicene, and (g) aminated silicene. Reprinted with permission from Ref. [105]. Copyright 2015 by Royal Society of Chemistry.

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Fig. 8.  (Color online) Preparation and photocurrent response of 2DSi-based devices. (a) Fabrication of photosensitive device based on silicane/polystyrene hybrids. (b, c) The plots of drain current versus time and drain current versus drain voltage of the devices fabricated following the procedures shown in (a). The inset in (c) shows a picture of the device setup under light irradiation. Reprinted with permission from Ref. [32]. Copyright 2017 by IOP Publishing Ltd.

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Fig. 9.  (Color online) Device architectures and performance of 2DSi-based optoelectronics. (a) Schematic illustration of the fabrication processes of the first silicene-based transistors with highlighted key steps. (b) Corresponding R versus Vg−Vdirac plot of silicene transistor showing the device evidence of the Dirac-like band structure of silicene. Reprinted with permission from Ref. [31]. Copyright 2015 by Macmillan Publishers Limited. (c) Device performance of SGFET using the hybrid active material containing dodecyl-functionalized silicane (SiNS-C12H25) and P3HT polymer. Inset: the schematic of the device architecture. (d) Output drain current-voltage curves of the device shown in Fig. (c). Inset: AFM image of the active layer. Reprinted with permission from Ref. [93]. Copyright 2017 by Wiley-VCH. (e) Device performance of SGFET based on silicane functionalized with various types of ligands: dodecane (C12H25), phenylacetylene (PhAC), and 2-ethinyl-3-hexylthiophene (ThAC). The device architecture is shown in the inset figure. Reprinted with permission from Ref. [87]. Copyright 2018 by Royal Society of Chemistry. (f) Schematic (top) and optical image (bottom) of the device architecture of phototransistor based on organo-modified silicanes (OMS)/graphene hybrids. (g) Corresponding IDS–VG curves of the devices with and without the presence of OMS. (h) Photocurrent response of the OMS/graphene hybrid phototransistors. Reprinted with permission from Ref. [107]. Copyright 2019 by Wiley-VCH.

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Fig. 10.  (Color online) 2DSi-based LEDs. (a) Transmission electron microscopic images and corresponding diffraction pattern (inset) of MSNs used for LED application. (b) Real color images of the thickness-controlled MSNs with emission ranging from blue to red and corresponding PL spectra as a function of growth time. (c) Optical bandgap of MSNs as a function of the thickness determined from PL and photocurrent measurements. Inset: the optical bandgap as a function of thickness. (d) Schematic of the hybrid LEDs using MSNs as the active materials. (e) Electroluminescence (EL) spectrum of the MSN-based devices using mixed MSNs with various thicknesses. (f) EL spectrum of the SiNSs synthesized for a growth time of 5 min. Reprinted with permission from Ref. [30]. Copyright 2014 by American Chemical Society.

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Table 1.   Summary of recently reported approaches to prepare 2DSi nanomaterials. Note: EG = epitaxial growth, CE = chemical exfoliation.

ProductYearSynthetic methodSilicon sourceLateral size (µm)Thickness (nm)Ref.
Silicene2012EG on Ag(111)Si wafer> 0.03–[29]
Silicene2013EG on Ir(111)Si wafer> 0.020.06[60]
Silicane2006CE of metal silicideCaSi1.85Mg0.150.2–0.50.37[66]
Silicane2018CE of metal silicideCaSi2~3.70.6[42]
MSN2014EG on Si substrateSiCl4–1–13[30]
MSN2014Arc dischargebulk Si0.022.4[57]
MSN2017EG on Ag(111)Si wafer> 0.057[47]
MSN2017CE of metal silicideLi13Si4~5.14[67]
MSN2018EG on NaCl substrateSiH4~5.250[58]
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    Received: 23 September 2022 Revised: 07 November 2022 Online: Accepted Manuscript: 17 November 2022Uncorrected proof: 18 November 2022Published: 10 April 2023

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      Article Navigation >  Journal of Semiconductors  > 2023  >  44(4): 041101
      Xuebiao Deng, Huai Chen, Zhenyu Yang. Two-dimensional silicon nanomaterials for optoelectronics[J]. Journal of Semiconductors, 2023, 44(4): 041101. doi: 10.1088/1674-4926/44/4/041101 ****Xuebiao Deng, Huai Chen, Zhenyu Yang. 2023: Two-dimensional silicon nanomaterials for optoelectronics. Journal of Semiconductors, 44(4): 041101. doi: 10.1088/1674-4926/44/4/041101
      Citation:
      Xuebiao Deng, Huai Chen, Zhenyu Yang. Two-dimensional silicon nanomaterials for optoelectronics[J]. Journal of Semiconductors, 2023, 44(4): 041101. doi: 10.1088/1674-4926/44/4/041101 ****
      Xuebiao Deng, Huai Chen, Zhenyu Yang. 2023: Two-dimensional silicon nanomaterials for optoelectronics. Journal of Semiconductors, 44(4): 041101. doi: 10.1088/1674-4926/44/4/041101
      shu

      Two-dimensional silicon nanomaterials for optoelectronics

      doi: 10.1088/1674-4926/44/4/041101

      • MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China

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      • Xuebiao Deng：received his bachelor’s degree from the School of Chemistry at Sun Yat-sen University in 2019. He is currently a Ph.D. candidate supervised by Professor Zhenyu Yang at Sun Yat-sen University. His research has focused on the synthesis and applications of two-dimensional silicon and germanium nanostructures
      • Huai Chen：earned his Ph.D. in Chemistry from Sun Yat-sen University in 2022. He has been working on his postdoctoral research at the School of Chemistry, Sun Yat-sen University. His current research interest includes silicon-based nanomaterials for biomedical and optoelectronic applications
      • Zhenyu Yang：received his B.Sc. degree in Chemistry from Nankai University in 2009 and his Ph.D. degree in Chemistry from the University of Alberta in 2014. From 2014 to 2018, he was a postdoctoral researcher at the University of Toronto. In 2018, he joined the School of Chemistry at Sun Yat-sen University as a Professor. His research focuses on the development of solution-processible optoelectronic materials and devices
      • Corresponding author: yangzhy63@mail.sysu.edu.cn
      • Received Date: 2022-09-23
      • Revised Date: 2022-11-07
        • Available Online: 2022-11-17

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