J. Semicond. > Volume 40 > Issue 6 > Article Number: 062001

Growth of oxidation-resistive silicene-like thin flakes and Si nanostructures on graphene

Naili Yue 1, , Joshua Myers 2, , Liqin Su 1, , Wentao Wang 3, , Fude Liu 3, , Raphael Tsu 1, , Yan Zhuang 2, and Yong Zhang 1, ,

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Abstract: We report the growth of Si nanostructures, either as thin films or nanoparticles, on graphene substrates. The Si nanostructures are shown to be single crystalline, air stable and oxidation resistive, as indicated by the observation of a single crystalline Si Raman mode at around 520 cm–1, a STM image of an ordered surface structure under ambient condition, and a Schottky junction with graphite. Ultra-thin silicon regions exhibit silicene-like behavior, including a Raman mode at around 550 cm–1, a triangular lattice structure in STM that has distinctly different lattice spacing from that of either graphene or thicker Si, and metallic conductivity of up to 500 times higher than that of graphite. This work suggests a bottom-up approach to forming a Si nanostructure array on a large-scale patterned graphene substrate that can be used to fabricate nanoscale Si electronic devices.

Key words: silicenesiliconRamanSTMepitaxial growthoxidation

Abstract: We report the growth of Si nanostructures, either as thin films or nanoparticles, on graphene substrates. The Si nanostructures are shown to be single crystalline, air stable and oxidation resistive, as indicated by the observation of a single crystalline Si Raman mode at around 520 cm–1, a STM image of an ordered surface structure under ambient condition, and a Schottky junction with graphite. Ultra-thin silicon regions exhibit silicene-like behavior, including a Raman mode at around 550 cm–1, a triangular lattice structure in STM that has distinctly different lattice spacing from that of either graphene or thicker Si, and metallic conductivity of up to 500 times higher than that of graphite. This work suggests a bottom-up approach to forming a Si nanostructure array on a large-scale patterned graphene substrate that can be used to fabricate nanoscale Si electronic devices.

Key words: silicenesiliconRamanSTMepitaxial growthoxidation



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Cinquanta E, Scalise E., Chiappe D, et al Getting through the nature of silicene: an sp2-sp3 two-dimensional silicon nanosheet. J Phys Chem C, 20113, 117, 16719

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Solonenko D, Gordan O, Lay G L, et al. 2D vibrational properties of epitaxial silicene on Ag(111). 2D Mater, 2017, 4, 015008

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Zhuang J, Xu X, Du Y, et al. Investigation of electron–phonon coupling in epitaxial silicene by in situ Raman spectroscopy. Phys Rev B, 2015, 91, 161409

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Sheng S, Wu J B, Cong X, et al. Vibrational properties of a monolayer silicene sheet studied by tip-enhanced Raman spectroscopy. Phys Rev Lett, 2017, 119, 196803

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Wu J B, Lin M L, Cong X, et al. Raman spectroscopy of graphene-based materials and its applications in related devices. Chem Soc Rev, 2018, 47, 1822

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De Padova P, Ottaviani C, Quaresima C, et al. 24 h stability of thick multilayer silicene in air. 2D Mater, 2014, 1, 021003

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Zhang Y, Tsu R. Binding graphene sheets together using silicon: graphene/silicon superlattice. Nanoscale Res Lett, 2010, 5, 805

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Neuendorf R, Palmer R E, Smith R. Low energy deposition of size-selected Si clusters onto graphite. Chem Phys Lett, 2001, 333, 304

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Cai Y, Chuu C P, Wei C M, et al. Stability and electronic properties of two-dimensional silicene and germanene on graphene. Phys Rev B, 2013, 88, 245408

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Yu S, Li X D, Wu S Q, et al. Novel electronic structures of superlattice composed of graphene and silicene. Mater Res Bull, 2014, 50, 268

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Wang J, Zhang Y. Topologic connection between 2-D layered structures and 3-D diamond structures for conventional semiconductors. Sci Rep, 2016, 6, 24660

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Zhang Y, Tsu R, Yue N. Growth of semiconductors on hetero-substrates using graphene as an interfacial layer. US Patent, US2014/039596, 2014

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De Crescenzi M, Berbezier I, Scarselli M, et al. Formation of silicene nanosheets on graphite. ACS Nano, 2016, 10, 11163

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Li Y, Wang H, Xie L, et al. MoS2 nanoparticles grown on graphene: an advanced catalyst for the hydrogen evolution reaction. J Am Cheml Soc, 2011, 133, 7296

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Ugeda M M, Bradley A J, Shi S F, et al. Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor. Nat Mater, 2014, 13, 1091

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Teplin C W, Paranthaman M P, Fanning T R, et al. Heteroepitaxial film crystal silicon on Al2O3: new route to inexpensive crystal silicon photovoltaics. Energy Environ Sci, 2011, 4, 3346

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Zhang K, Seo J H, Zhou W D, et al. Fast flexible electronics using transferrable silicon nanomembranes. J Phys D, 2012, 45, 143001

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Wang L, Tu H L, Zhu S W, et al. Dispersed Si nanoparticles with narrow photoluminescence peak prepared by laser ablated deposition. Chin J Nonferrous Metals, 2010, 20, 724

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Baba Y, Shimoyama I, Hirao N, et al. Structure of ultra-thin silicon film on HOPG studied by polarization-dependence of X-ray absorption fine structure. Chem Phys Lett, 2014, 594, 64

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Evanoff K, Magasinski A, Yang J, et al. Nanosilicon-coated graphene granules as anodes for Li-ion batteries. Adv Energy Mater, 2011, 1, 495

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Su L, Zhang Y, Yu Y, et al. Dependence of coupling of quasi 2-D MoS2 with substrates on substrate types, probed by temperature dependent Raman scattering. Nanoscale, 2014, 6, 4920

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Su L, Yu Y, Cao L, et al. Effects of substrate type and material-substrate bonding on high-temperature behavior of monolayer WS2. Nano Res, 2015, 8, 2686

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Su L, Yu Y, Cao L, et al. In situ in situ monitoring of the thermal-annealing effect in a monolayer of MoS2. Phys Rev Appl, 2017, 7, 034009

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Li L X, Han W P, Wu W. J B, et al Layer-number dependent optical properties of 2D materials and their application for thickness determination. Adv Funct Mater, 2017, 27, 1604468

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Malinovsky V K, Novikov V N, Surovtsev N V, et al. Investigation of amorphous states of SiO2 by Raman scattering spectroscopy. Phys Solid State, 2000, 42, 65

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Ivanda M, Clasen R, Hornfeck M, et al. Raman spectroscopy on SiO2 glasses sintered from nanosized particles. J Non-Cryst Solids, 2003, 322, 46

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Raider S I, Flitsch R, Palmer M J. Oxide growth on etched silicon in air at room temperature. J Electrochem Soc, 1975, 122, 413

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Ryckman J D, Reed R A, Weller R A, et al. Enhanced room temperature oxidation in silicon and porous silicon under 10 keV X-ray irradiation. J Appl Phys, 2010, 108, 113528

[39]

Tongay S, Schumann T, Hebard A F. Graphite based Schottky diodes formed on Si, GaAs, and 4H-SiC substrates. Appl Phys Lett, 2009, 95, 222103

[40]

Sinha D, Lee J U. Ideal graphene/silicon schottky junction diodes. Nano Lett, 2014, 14, 4660

[41]

Riazimehr S, Schneider D, Yim C, et al. Spectral sensitivity of a graphene/silicon pn-junction photodetector. 2015 Joint International EUROSOI Workshop and International Conference on Ultimate Integration on Silicon, 2015, 77

[42]

Guo Z X, Zhang Y Y, Xiang H, et al. Structural evolution and optoelectronic applications of multilayer silicene. Phys Rev B, 2015, 92, 201413

[43]

Mizes H A, Park S I, Harrison W A. Multiple-tip interpretation of anomalous scanning-tunneling-microscopy images of layered materials. Phys Rev B, 1987, 36, 4491

[44]

Hembacher S, Giessibl F J, Mannhart J, et al. Revealing the hidden atom in graphite by low-temperature atomic force microscopy. Proc Natl Acad Sci, 2003, 100, 12539

[45]

Neddermeyer H. Scanning tunnelling microscopy of semiconductor surfaces. Rep Prog Phys, 1996, 59, 701

[46]

Zhang Y, Dalpian G M, Fluegel B, et al. Novel approach to tuning the physical properties of organic-inorganic hybrid semiconductors. Phys Rev Lett, 2006, 96, 026405

[47]

Yue N, Zhang Y, Tsu R. Ambient condition laser writing of graphene structures on polycrystalline SiC thin film deposited on Si wafer. Appl Phys Lett, 2013, 102, 071912

[1]

Guzm-Verri G G, Lew Yan Voon L C. Electronic structure of silicon-based nanostructures. Phys Rev B, 2007, 76, 075131

[2]

Vogt P, De Padova P, Quaresima C, et al. Silicene: compelling experimental evidence for graphenelike two-dimensional silicon. Phys Rev Lett, 2012, 108, 155501

[3]

Fleurence A, Friedlein R, Ozaki T, et al. Experimental evidence for epitaxial silicene on diboride thin Films. Phys Rev Lett, 2012, 108, 245501

[4]

Cinquanta E, Scalise E., Chiappe D, et al Getting through the nature of silicene: an sp2-sp3 two-dimensional silicon nanosheet. J Phys Chem C, 20113, 117, 16719

[5]

Yan J A, Stein R, Schaefer D M, et al. Electron-phonon coupling in two-dimensional silicene and germanene. Phys Rev B, 2013, 88, 121403

[6]

Scalise E, Houssa M, Pourtois G, et al. Vibrational properties of silicene and germanene. Nano Res, 2013, 6, 19

[7]

Solonenko D, Gordan O, Lay G L, et al. 2D vibrational properties of epitaxial silicene on Ag(111). 2D Mater, 2017, 4, 015008

[8]

Zhuang J, Xu X, Du Y, et al. Investigation of electron–phonon coupling in epitaxial silicene by in situ Raman spectroscopy. Phys Rev B, 2015, 91, 161409

[9]

Sheng S, Wu J B, Cong X, et al. Vibrational properties of a monolayer silicene sheet studied by tip-enhanced Raman spectroscopy. Phys Rev Lett, 2017, 119, 196803

[10]

Wu J B, Lin M L, Cong X, et al. Raman spectroscopy of graphene-based materials and its applications in related devices. Chem Soc Rev, 2018, 47, 1822

[11]

De Padova P, Ottaviani C, Quaresima C, et al. 24 h stability of thick multilayer silicene in air. 2D Mater, 2014, 1, 021003

[12]

Zhang Y, Tsu R. Binding graphene sheets together using silicon: graphene/silicon superlattice. Nanoscale Res Lett, 2010, 5, 805

[13]

Neuendorf R, Palmer R E, Smith R. Low energy deposition of size-selected Si clusters onto graphite. Chem Phys Lett, 2001, 333, 304

[14]

Cai Y, Chuu C P, Wei C M, et al. Stability and electronic properties of two-dimensional silicene and germanene on graphene. Phys Rev B, 2013, 88, 245408

[15]

Yu S, Li X D, Wu S Q, et al. Novel electronic structures of superlattice composed of graphene and silicene. Mater Res Bull, 2014, 50, 268

[16]

Fahy S, Louie S G, Cohen M L. Pseudopotential total-energy study of the transition from rhombohedral graphite to diamond. Phys Rev B, 1986, 34, 1191

[17]

Wang J, Zhang Y. Topologic connection between 2-D layered structures and 3-D diamond structures for conventional semiconductors. Sci Rep, 2016, 6, 24660

[18]

Zhang Y, Tsu R, Yue N. Growth of semiconductors on hetero-substrates using graphene as an interfacial layer. US Patent, US2014/039596, 2014

[19]

De Crescenzi M, Berbezier I, Scarselli M, et al. Formation of silicene nanosheets on graphite. ACS Nano, 2016, 10, 11163

[20]

Li Y, Wang H, Xie L, et al. MoS2 nanoparticles grown on graphene: an advanced catalyst for the hydrogen evolution reaction. J Am Cheml Soc, 2011, 133, 7296

[21]

Ugeda M M, Bradley A J, Shi S F, et al. Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor. Nat Mater, 2014, 13, 1091

[22]

Teplin C W, Paranthaman M P, Fanning T R, et al. Heteroepitaxial film crystal silicon on Al2O3: new route to inexpensive crystal silicon photovoltaics. Energy Environ Sci, 2011, 4, 3346

[23]

Zhang K, Seo J H, Zhou W D, et al. Fast flexible electronics using transferrable silicon nanomembranes. J Phys D, 2012, 45, 143001

[24]

Marsen B, Sattler K. Fullerene-structured nanowires of silicon. Phys Rev B, 1999, 60, 11593

[25]

Nath K G, Shimoyama I, Sekiguchi T, et al. Chemical-state analysis for low-dimensional Si and Ge films on graphite. J Appl Phys, 2003, 94, 4583

[26]

Kunze T, Hauttmann S, Seekamp J, et al. Recrystallized and epitaxially thickened poly-silicon layers on graphite substrates. Conference Record of the IEEE Photovoltaic Specialists Conference, 1997, 735

[27]

Beaucarne G, Bourdais S, Slaoui A, et al. Impurity diffusion from uncoated foreign substrates during high temperature CVD for thin-film Si solar cells. Sol Energy Mater Sol Cells, 2000, 61, 301

[28]

Wang L, Tu H L, Zhu S W, et al. Dispersed Si nanoparticles with narrow photoluminescence peak prepared by laser ablated deposition. Chin J Nonferrous Metals, 2010, 20, 724

[29]

Baba Y, Shimoyama I, Hirao N, et al. Structure of ultra-thin silicon film on HOPG studied by polarization-dependence of X-ray absorption fine structure. Chem Phys Lett, 2014, 594, 64

[30]

Evanoff K, Magasinski A, Yang J, et al. Nanosilicon-coated graphene granules as anodes for Li-ion batteries. Adv Energy Mater, 2011, 1, 495

[31]

Su L, Zhang Y, Yu Y, et al. Dependence of coupling of quasi 2-D MoS2 with substrates on substrate types, probed by temperature dependent Raman scattering. Nanoscale, 2014, 6, 4920

[32]

Su L, Yu Y, Cao L, et al. Effects of substrate type and material-substrate bonding on high-temperature behavior of monolayer WS2. Nano Res, 2015, 8, 2686

[33]

Su L, Yu Y, Cao L, et al. In situ in situ monitoring of the thermal-annealing effect in a monolayer of MoS2. Phys Rev Appl, 2017, 7, 034009

[34]

Li L X, Han W P, Wu W. J B, et al Layer-number dependent optical properties of 2D materials and their application for thickness determination. Adv Funct Mater, 2017, 27, 1604468

[35]

Malinovsky V K, Novikov V N, Surovtsev N V, et al. Investigation of amorphous states of SiO2 by Raman scattering spectroscopy. Phys Solid State, 2000, 42, 65

[36]

Ivanda M, Clasen R, Hornfeck M, et al. Raman spectroscopy on SiO2 glasses sintered from nanosized particles. J Non-Cryst Solids, 2003, 322, 46

[37]

Raider S I, Flitsch R, Palmer M J. Oxide growth on etched silicon in air at room temperature. J Electrochem Soc, 1975, 122, 413

[38]

Ryckman J D, Reed R A, Weller R A, et al. Enhanced room temperature oxidation in silicon and porous silicon under 10 keV X-ray irradiation. J Appl Phys, 2010, 108, 113528

[39]

Tongay S, Schumann T, Hebard A F. Graphite based Schottky diodes formed on Si, GaAs, and 4H-SiC substrates. Appl Phys Lett, 2009, 95, 222103

[40]

Sinha D, Lee J U. Ideal graphene/silicon schottky junction diodes. Nano Lett, 2014, 14, 4660

[41]

Riazimehr S, Schneider D, Yim C, et al. Spectral sensitivity of a graphene/silicon pn-junction photodetector. 2015 Joint International EUROSOI Workshop and International Conference on Ultimate Integration on Silicon, 2015, 77

[42]

Guo Z X, Zhang Y Y, Xiang H, et al. Structural evolution and optoelectronic applications of multilayer silicene. Phys Rev B, 2015, 92, 201413

[43]

Mizes H A, Park S I, Harrison W A. Multiple-tip interpretation of anomalous scanning-tunneling-microscopy images of layered materials. Phys Rev B, 1987, 36, 4491

[44]

Hembacher S, Giessibl F J, Mannhart J, et al. Revealing the hidden atom in graphite by low-temperature atomic force microscopy. Proc Natl Acad Sci, 2003, 100, 12539

[45]

Neddermeyer H. Scanning tunnelling microscopy of semiconductor surfaces. Rep Prog Phys, 1996, 59, 701

[46]

Zhang Y, Dalpian G M, Fluegel B, et al. Novel approach to tuning the physical properties of organic-inorganic hybrid semiconductors. Phys Rev Lett, 2006, 96, 026405

[47]

Yue N, Zhang Y, Tsu R. Ambient condition laser writing of graphene structures on polycrystalline SiC thin film deposited on Si wafer. Appl Phys Lett, 2013, 102, 071912

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N L Yue, J Myers, L Q Su, W T Wang, F D Liu, R Tsu, Y Zhuang, Y Zhang, Growth of oxidation-resistive silicene-like thin flakes and Si nanostructures on graphene[J]. J. Semicond., 2019, 40(6): 062001. doi: 10.1088/1674-4926/40/6/062001.

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Manuscript received: 05 February 2019 Manuscript revised: 01 March 2019 Online: Accepted Manuscript: 23 April 2019 Uncorrected proof: 26 April 2019 Published: 05 June 2019

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