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在分子束外延(MBE)设备中,利用直接沉积C原子的方法在覆盖有SiO2的Si衬底(SiO2/Si)上生长石墨烯,并通过Raman光谱和近边X射线吸收精细结构谱等实验技术对不同衬底温度(500℃,600℃,700℃,900℃,1100℃,1200℃)生长的薄膜进行结构表征.实验结果表明,在衬底温度较低时生长的薄膜是无定形碳,在衬底温度高于700℃时薄膜具有石墨烯的特征,而且石墨烯的结晶质量随着衬底温度的升高而改善,但过高的衬底温度会使石墨烯质量降低.衬底温度为1100℃时结晶质量最好.衬底温度较低时C原子活性较低,难以形成有序的C-sp2六方环.而衬底温度过高时(1200℃),衬底表面部分SiO2分解,C原子与表面的Si原子或者O原子结合而阻止石墨烯的形成,并产生表面缺陷导致石墨烯结晶变差.Graphene thin films are grown on Si substrates covered by SiO2 layers (SiO2/Si) with the method of directly depositing carbon atoms in the molecular beam epitaxy (MBE) equipment. The structural properties of the samples produced at different substrate temperatures (500℃, 600℃, 900℃, 1100℃, 1200℃) are investigated by Raman spectroscopy (Raman) and near-edge x-ray absorption fine structure (NEXAFS). The results indicate that the thin films grown at lower temperatures are amorphous carbon thin films. While the thin films grown above 700℃ exhibi the characteristics of graphene. As the substrate temperature increases, the crystalline quality of graphene is improved. However, very high temperature can reduce the quality of grapheme. The best graphene films are obtained at a substrate temperature of 1100℃. When the substrate temperature is low, the activity of the carbon atoms is not enough to form the ordered six member rings of C-sp2. While the substrate temperature is too high, the decomposition of some SiO2 induces the deposited carbon atoms to bond with decomposed oxygen atoms or silicon atoms, resulting in the defects on the surface, which leads to the poor crystalline quality of graphene films.
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Keywords:
- MBE /
- graphene /
- SiO2Si /
- synchrotron radiation
[1] Novoselov K S, Geim A K, Firsov A A 2004 Science 306 666
[2] Xu X G, Zhang C , Xu G J, Cao J C 2011 Chin. Phys. B 20 027201
[3] Service R F 2009 Science 324 875
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[7] Berger C, Song Z, Li T, Li X, Ogbazghi A Y, Feng R, Dai Z, Marchenkov A N, Conrad E H, First P N, de HeerW2004 J. Phys.Chemi. B 108 19912
[8] Tang C, Ji L, Meng L J, Sun L Z, Zhang K W, Zhong J X 2009Acta Phys. Sin. 58 7816 (in Chinese) [唐超, 吉璐, 孟利军, 孙立忠, 张凯旺, 钟建新 2009 58 7816]
[9] Stankovich S, Dikin D A, Dommett G H B, Kohlhaas K M, ZimneyE J, Stach E A, Piner R D, Nguyen S T, Ruoff R S 2006 Nature442 282
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[12] Hackley J, Ali D, DiPasquale J, Demaree J D, Richardson C J K2009 Appl. Phys. Lett. 95 133114
[13] Ouerghi A, Kahouli A, Lucot D, Portail M, Travers L, Gierak J, Penuelas, Jegou P, Shukla A, Chassagne T, ZielinskiM2010 Appl.Phys. Lett. 96 191910
[14] Suemitsu M, Fukidome H 2010 J. Phys. D: Appl. Phys. 43 374012
[15] Park J, Mitchel W C, Grazulis L, Smith H E, Eyink K G, BoecklJ J, Tomich D H, Pacley S D, Hoelscher J E 2010 Adv. Mater. 224140
[16] Tang J, Kang C Y, Li L M, Yan W S, Wei S Q, Xu P S 2011Physica E 43 1415
[17] Ni Z H, Chen W, Fan X F, Kuo J L, Yu T, Wee A T S, Shen Z X2008 Phys. Rev. B 77 115416
[18] Röhrl J, Hundhausen M, Emtsev K V, Seyller T, Graupner R, LeyL 2008 Appl. Phys. Lett. 92 01918
[19] Thomsen C, Reich S 2000 Phys. Rev. Lett. 85 5214
[20] Chen D W 2010 Acta Phys. Sin. 59 6399 (in Chinese) [陈东猛 2010 59 6399]
[21] Pimenta M A, Dresselhaus G, Dresselhaus M S, Cancado L G, Jorioa A, Saito R 2007 Phys. Chem. Chem. Phys. 9 1276
[22] Ferralis N, Maboudian R, Carraro C 2008 Phys. Rev. Lett. 101156801
[23] Canc?ado L G, Takai K, Enoki T, Endo M, Kim Y A, Mizusaki H, Jorio A, Coelho L N, Magalh?aes-Paniago R, Pimenta M A 2006Appl. Phys. Lett. 88 163106
[24] Ferrari A C, Meyer J C, Scardaci V, Casiraghi C, Lazzeri M, MauriF, Piscanec S, Jiang D, Novoselov K S, Roth S, Geim A K 2006Phys. Phys. Rev. Lett. 97 187401
[25] Ferrari A C, Robertson J, Tan P H, Li F, Cheng H M translated2007 Raman Spectroscopy in Carbons: from Nanotubes to Diamondpp4–23 (in Chinese) [德里亚·卡罗·费拉里, 约翰·罗伯逊编, 谭平恒, 李峰, 成会明 译 2007 碳材料的拉曼光谱——-从纳米管到金刚石 (北京: 化学工业出版社), 第4——23页]
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[27] Malarda L M, Pimentaa M A, Dresselhaus G, Dresselhaus M S2009 Phys. Rep. 473 51
[28] Faugeras C, Nerrire A, Potemski M, Mahmood A, Dujardin E, Berger C, de Heer W A 2008 Appl. Phys. Lett. 92 011914
[29] Tang J, Liu Z L, Ren P, Yao T, Yan W S, Xu P S , Wei S Q 2010Acta Phys. Sin. 59 372 (in Chinese) [唐军, 刘忠良, 任鹏, 姚涛, 闫文盛, 徐彭寿, 韦世强 2010 59 372]
[30] Batson P E 1993 Phys. Rev. B 48 2608
[31] Fischer D A, Wentzcovitch R M, Carr R G, Continenza A, FreemanA J 1991 Phys. Rev. B 44 1427
[32] Abbas M, Wu Z Y, Zhong J, Ibrahim K, Fiori A, Orlanducci S, Sessa V, TerranovaML, Ivan D 2005 Appl. Phys. Lett. 87 051923
[33] Jeong H K, Colakerol L, Jin M H, Glans P A, Smith K E, Lee YH 2008 Chem. Phys. Lett. 460 499
[34] Emtsev K V, Speck F, Seyller Th, Ley L 2008 Phys. Rev. B 77155303
[35] Konya Z, Vesselenyi I, Kiss J, Farkas A, Oszko A 2004 Appl.Catalysis A: Grneral 260 55037302-6
-
[1] Novoselov K S, Geim A K, Firsov A A 2004 Science 306 666
[2] Xu X G, Zhang C , Xu G J, Cao J C 2011 Chin. Phys. B 20 027201
[3] Service R F 2009 Science 324 875
[4] Morzov S V, Novoselov K S, Katsnelson M I, Schedin F, Elias DC, Jaszczak J A, Geim A K 2008 Phys. Rev. Lett. 100 016602
[5] Balandin A A, Ghosh S, BaoWZ, Calizo I, Teweldebrhan D, MiaoF, Lau C N 2008 Nano Lett. 8 902
[6] Kang C Y, Tang J, Li L M, Pan H B, Yan W S, Xu P S, Wei S Q, Chen X F, Xu X G 2011 Acta Phys. Sin. 60 047302 (in Chinese)康朝阳, 唐军, 李利民, 潘海斌, 闫文盛, 徐彭寿, 韦世强, 陈秀芳, 徐现刚 2011 60 047302]
[7] Berger C, Song Z, Li T, Li X, Ogbazghi A Y, Feng R, Dai Z, Marchenkov A N, Conrad E H, First P N, de HeerW2004 J. Phys.Chemi. B 108 19912
[8] Tang C, Ji L, Meng L J, Sun L Z, Zhang K W, Zhong J X 2009Acta Phys. Sin. 58 7816 (in Chinese) [唐超, 吉璐, 孟利军, 孙立忠, 张凯旺, 钟建新 2009 58 7816]
[9] Stankovich S, Dikin D A, Dommett G H B, Kohlhaas K M, ZimneyE J, Stach E A, Piner R D, Nguyen S T, Ruoff R S 2006 Nature442 282
[10] Di C A, Wei D C, Yu G, Liu Y Q, Guo Y L, Zhu D B 2008 Adv.Mater. 20 3289
[11] Wu J S, Pisula W, Mullen K 2007 Chem. Rev. 107 718
[12] Hackley J, Ali D, DiPasquale J, Demaree J D, Richardson C J K2009 Appl. Phys. Lett. 95 133114
[13] Ouerghi A, Kahouli A, Lucot D, Portail M, Travers L, Gierak J, Penuelas, Jegou P, Shukla A, Chassagne T, ZielinskiM2010 Appl.Phys. Lett. 96 191910
[14] Suemitsu M, Fukidome H 2010 J. Phys. D: Appl. Phys. 43 374012
[15] Park J, Mitchel W C, Grazulis L, Smith H E, Eyink K G, BoecklJ J, Tomich D H, Pacley S D, Hoelscher J E 2010 Adv. Mater. 224140
[16] Tang J, Kang C Y, Li L M, Yan W S, Wei S Q, Xu P S 2011Physica E 43 1415
[17] Ni Z H, Chen W, Fan X F, Kuo J L, Yu T, Wee A T S, Shen Z X2008 Phys. Rev. B 77 115416
[18] Röhrl J, Hundhausen M, Emtsev K V, Seyller T, Graupner R, LeyL 2008 Appl. Phys. Lett. 92 01918
[19] Thomsen C, Reich S 2000 Phys. Rev. Lett. 85 5214
[20] Chen D W 2010 Acta Phys. Sin. 59 6399 (in Chinese) [陈东猛 2010 59 6399]
[21] Pimenta M A, Dresselhaus G, Dresselhaus M S, Cancado L G, Jorioa A, Saito R 2007 Phys. Chem. Chem. Phys. 9 1276
[22] Ferralis N, Maboudian R, Carraro C 2008 Phys. Rev. Lett. 101156801
[23] Canc?ado L G, Takai K, Enoki T, Endo M, Kim Y A, Mizusaki H, Jorio A, Coelho L N, Magalh?aes-Paniago R, Pimenta M A 2006Appl. Phys. Lett. 88 163106
[24] Ferrari A C, Meyer J C, Scardaci V, Casiraghi C, Lazzeri M, MauriF, Piscanec S, Jiang D, Novoselov K S, Roth S, Geim A K 2006Phys. Phys. Rev. Lett. 97 187401
[25] Ferrari A C, Robertson J, Tan P H, Li F, Cheng H M translated2007 Raman Spectroscopy in Carbons: from Nanotubes to Diamondpp4–23 (in Chinese) [德里亚·卡罗·费拉里, 约翰·罗伯逊编, 谭平恒, 李峰, 成会明 译 2007 碳材料的拉曼光谱——-从纳米管到金刚石 (北京: 化学工业出版社), 第4——23页]
[26] Gupta A, Chen G, Joshi P, Tadigadapa S, Eklund P C 2006 NanoLett. 6 2667
[27] Malarda L M, Pimentaa M A, Dresselhaus G, Dresselhaus M S2009 Phys. Rep. 473 51
[28] Faugeras C, Nerrire A, Potemski M, Mahmood A, Dujardin E, Berger C, de Heer W A 2008 Appl. Phys. Lett. 92 011914
[29] Tang J, Liu Z L, Ren P, Yao T, Yan W S, Xu P S , Wei S Q 2010Acta Phys. Sin. 59 372 (in Chinese) [唐军, 刘忠良, 任鹏, 姚涛, 闫文盛, 徐彭寿, 韦世强 2010 59 372]
[30] Batson P E 1993 Phys. Rev. B 48 2608
[31] Fischer D A, Wentzcovitch R M, Carr R G, Continenza A, FreemanA J 1991 Phys. Rev. B 44 1427
[32] Abbas M, Wu Z Y, Zhong J, Ibrahim K, Fiori A, Orlanducci S, Sessa V, TerranovaML, Ivan D 2005 Appl. Phys. Lett. 87 051923
[33] Jeong H K, Colakerol L, Jin M H, Glans P A, Smith K E, Lee YH 2008 Chem. Phys. Lett. 460 499
[34] Emtsev K V, Speck F, Seyller Th, Ley L 2008 Phys. Rev. B 77155303
[35] Konya Z, Vesselenyi I, Kiss J, Farkas A, Oszko A 2004 Appl.Catalysis A: Grneral 260 55037302-6
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