多層グラフェン薄膜の乱層構造に起因する特異物性の研究

• Project Area: Materials Science and Advanced Elecronics created by singularity
• Project/Area Number: 17H05336
• Research Category: Grant-in-Aid for Scientific Research on Innovative Areas (Research in a proposed research area)
• Allocation Type: Single-year Grants
• Review Section: Science and Engineering
• Research Institution: Osaka University
• Principal Investigator: 小林 慶裕 大阪大学, 工学研究科, 教授 (30393739)
• Project Period (FY): 2017-04-01 – 2019-03-31
• Project Status: Completed (Fiscal Year 2018)
• Budget Amount: ¥4,030,000 (Direct Cost: ¥3,100,000、Indirect Cost: ¥930,000); Fiscal Year 2018: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000); Fiscal Year 2017: ¥1,950,000 (Direct Cost: ¥1,500,000、Indirect Cost: ¥450,000)
• Keywords: 乱層構造 / グラフェン / 酸化グラフェン / 超高温プロセス / 欠陥修復 / キャリア輸送特性 / 熱伝導特性 / ナノ材料 / 結晶工学 / 薄膜物性

Outline of Annual Research Achievements

本研究では、大量製造可能な酸化グラフェン(GO)から反応性雰囲気での超高温処理により低欠陥・乱層・多層グラフェン薄膜を形成し、そこから単層に類似した優れた特性を引き出して乱層構造の物性優位性を検証することを目的とする。今年度は、本研究の１年目で見出した成果、すなわち高空隙スポンジ状GOの超高温処理による低欠陥・乱層グラフェンのスケーラブル形成を発展させ、物性計測に適した試料構造の作製を試みた。さらに乱層グラフェン試料を用いた物性評価を推し進め、炭素材料における特異構造である乱層構造から単層に類似した優れた物性を発現させる可能性について検証した。
物性解析に向けた薄膜試料作製法として、まずGO分散液を凍結乾燥して得られる自立構造体である多孔質GOスポンジを超高温で処理して、低欠陥・多層の３次元グラフェン集積体を作製した。このグラフェン構造体を100t以上の高圧で薄膜状に圧縮成型することを試みたが、この圧力でも弾性変形し、元の形状が維持されることが判明した。そのため、多孔質GOスポンジはそのままの形状を活かして電気化学電極としての性能検証へと展開することとした。物性解析試料の代替として、吸引濾過による薄膜形成法の検討を進めるとともに、化学気相法を用いて石英基板上に乱層グラフェンを形成する手法を開発した。得られた乱層グラフェン薄膜をチャネルとして電界効果トランジスタやホール素子を作製し、キャリア輸送特性を解析した。得られたキャリア移動度・密度などについてグラフェン層数・測定温度依存性を解析した結果、単層類似の輸送特性や基板近傍グラフェン層によるスクリーニング効果を明らかにした。この結果は、乱層構造を持つ多層グラフェンの物性的な優位性を示しており、今後の応用展開が期待される。

Research Progress Status

平成30年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

平成30年度が最終年度であるため、記入しない。

Research Products

• [Journal Article] Turbostratic multilayer graphene synthesis on CVD graphene template toward improving electrical performance (2019)
  • Author(s): Chaopeng Wei, Ryota Negishi, Yui Ogawa, Masashi Akabori, Yoshikata Taniyasu and Yoshihiro Kobayashi
  • Journal Title: Japanese Journal of Applied Physics Volume: 印刷中
  • NAID: 210000156355
  • Peer Reviewed
• [Journal Article] Effect of protective layer on CNT thin film channel in biosensor device (2019)
  • Author(s): Ritsu Niimi, Ryota Negishi, Michiharu Arifuku, Noriko Kiyoyanagi,Tomohiro Yamaguchi, Koji Ishibashi and Yoshihiro Kobayashi
  • Journal Title: Japanese Journal of Applied Physics Volume: 印刷中
  • Peer Reviewed
• [Journal Article] Neuromorphic Switching Behavior in the Multi-stacking Composed of Pt/Graphene Oxide/Ag2S/Ag (2019)
  • Author(s): Bruno Kenichi Saika, Ryota Negishi and Yoshihiro Kobayashi
  • Journal Title: Japanese Journal of Applied Physics Volume: 印刷中
  • NAID: 210000156684
  • Peer Reviewed
• [Journal Article] Investigation of surface potentials in reduced graphene oxide flake by Kelvin probe force microscopy (2018)
  • Author(s): Ryota Negishi, Kai Takashima and Yoshihiro Kobayashi
  • Journal Title: Japanese Journal of Applied Physics Volume: 57 Issue: 6S1 Pages: 06HD02-06HD02
  • DOI: 10.7567/jjap.57.06hd02
  • NAID: 210000149153
  • Peer Reviewed
• [Journal Article] Biosensor response from target molecules with inhomogeneous charge localization (2018)
  • Author(s): Hiroto Kase, Ryota Negishi, Michiharu Arifuku, Noriko Kiyoyanagi,Yoshihiro Kobayashi
  • Journal Title: Journal of Applied Physics Volume: 124 Issue: 6 Pages: 0645021-6
  • DOI: 10.1063/1.5036538
  • Peer Reviewed
• [Journal Article] Investigation of surface potentials in reduced graphene oxide flake by Kelvin probe force microscope (2018)
  • Author(s): Ryota Negishi,Kai Takashima and Yoshihiro Kobayashi
  • Journal Title: Japanese Journal of Applied Physics Volume: 印刷中
  • Peer Reviewed
• [Journal Article] Diameter dependence of longitudinal unzipping of single-walled carbon nanotube to obtain graphene nanoribbon (2017)
  • Author(s): Minoru Fukumori, Pandey Reetu Raj, Taizo Fujiwara, Amin TermehYousefi, Ryota Negishi, Yoshihiro Kobayashi, Hirofumi Tanaka, Takuji Ogawa
  • Journal Title: Japanese Jornal of Applied Physics Special issue Volume: 56 Issue: 6S1 Pages: 06GG12-06GG12
  • DOI: 10.7567/jjap.56.06gg12
  • Peer Reviewed
• [Journal Article] Synthesis of very narrow multilayer graphene nanoribbon with turbostratic stacking (2017)
  • Author(s): Negishi R.、Yamamoto K.、Kitakawa H.、Fukumori M.、Tanaka H.、Ogawa T.、Kobayashi Y.
  • Journal Title: Applied Physics Letters Volume: 110 Issue: 20 Pages: 201901-201901
  • DOI: 10.1063/1.4983349
  • Peer Reviewed
• [Journal Article] Improving sensor response using reduced graphene oxide film transistor biosensor by controlling the pyrene adsorption as an anchor molecules (2017)
  • Author(s): Ryota Negishi, Yuji Matsui and Yoshihiro Kobayashi
  • Journal Title: Japanese Jornal of Applied Physics Special issue Volume: 56 Issue: 6S1 Pages: 06GE04-06GE04
  • DOI: 10.7567/jjap.56.06ge04
  • Peer Reviewed
• [Journal Article] Synthesis of highly crystalline graphene films showing band-like transport from the defective graphene oxide (2017)
  • Author(s): 根岸 良太、小林 慶裕
  • Journal Title: ナノ学会会報 Volume: 15 Pages: 39-45
  • NAID: 40021178173
• [Journal Article] 酸化グラフェンからの高結晶性グラフェン薄膜の合成とバイオセンサー応用 (2017)
  • Author(s): 根岸 良太、小林 慶裕
  • Journal Title: MATERIAL STAGE Volume: 17 Pages: 1-6
• [Presentation] セルロースナノファイバー添加によるグラフェン積層構造への影響と熱伝導解析 (2019)
  • Author(s): 石黒 稚可子、許 梓釗、仁科 勇太、小林 慶裕
  • Organizer: ２０１９年第66回応用物理学会春季学術講演会
• [Presentation] グラフェンテンプレート上に合成した多層グラフェンのキャリア伝導特性 (2019)
  • Author(s): 根岸 良太、魏 超鵬、小川 友以、赤堀 誠志、谷保 芳孝、小林 慶裕
  • Organizer: ２０１９年第66回応用物理学会春季学術講演会
• [Presentation] Modulation of the resistance switching behavior of Ag2S-based switches using graphene oxide layer (2019)
  • Author(s): Bruno Kenichi Saika、Ryota Negishi、Yoshihiro Kobayashi
  • Organizer: ２０１９年第66回応用物理学会春季学術講演会
• [Presentation] Scalable synthesis of highly porous graphene with turbostratic stacking by thermal process of graphene oxide sponge (2018)
  • Author(s): Shingo Nakamura, Zizhao Xu, Yuta Nishina, Yoshihiro Kobayashi
  • Organizer: E-MRS 2018 Spring Meeting
  • Int'l Joint Research
• [Presentation] Restoration and layer-by-layer growth of graphene structures by controlling partial pressure of ethanol vapor through high process temperature (2018)
  • Author(s): R. Negishi and Y. Kobayashi
  • Organizer: Nanotech Malaysia 2018
  • Int'l Joint Research / Invited
• [Presentation] Scalable synthesis of highly porous nanocarbon materials by ultrahigh temperature process for graphene oxide and cellulose nanofiber composites (2018)
  • Author(s): Z. Xu, S. Nakamura, Y. Nishina, and Y. Kobayashi
  • Organizer: 19th Int. Conf. on the Sci. and Appl. of Nanotubes and Low-dimensional Materials
  • Int'l Joint Research
• [Presentation] Control of 12C/13C isotope in CNT grown from nanodiamond (2018)
  • Author(s): K. Nakamura, A. Ohhata, M. Arifuku, N. Kiyoyanagi, and Y. Kobayashi
  • Organizer: 19th Int. Conf. on the Sci. and Appl. of Nanotubes and Low-dimensional Materials
  • Int'l Joint Research
• [Presentation] valuation of electrical conductivity in turbostratic multilayer graphene films synthesized from CVD graphene (2018)
  • Author(s): C. Wei, R. Negishi, Y. Ogawa, M. Takamura, Y. Taniyasu, and Y. Kobayashi
  • Organizer: 19th Int. Conf. on the Sci. and Appl. of Nanotubes and Low-dimensional Materials
  • Int'l Joint Research
• [Presentation] Noise reduction in sensor response of carbon nanotube thin film biosensor using HfO2 layer as protective film (2018)
  • Author(s): R. Niimi, R. Negishi, M. Arifuku, N. Kiyoyanagi, T. Yamaguchi, K. Ishibashi and Y. Kobayashi
  • Organizer: 19th Int. Conf. on the Sci. and Appl. of Nanotubes and Low-dimensional Materials
  • Int'l Joint Research
• [Presentation] Synthesis of highly crystalline multilayer graphene on graphene template by high growth temperature (2018)
  • Author(s): R. Negishi, M. Maruoka, Y. Ogawa, M. Takamura, Y. Taniyasu, and Y. Kobayashi
  • Organizer: 19th Int. Conf. on the Sci. and Appl. of Nanotubes and Low-dimensional Materials
  • Int'l Joint Research
• [Presentation] Neuromorphic Switching Behavior in the Multi-stacking Composed of Ag/Ag2S/GO (2018)
  • Author(s): B. K. Saika, R. Negishi and Y. Kobayashi
  • Organizer: 14th Int. Conf. on Atomically Controlled Surfaces, Interfaces and Nanostructures (ACSIN-14)
  • Int'l Joint Research
• [Presentation] Effect of protective layer on CNT thin film channel in biosensor device (2018)
  • Author(s): R. Niimi, R. Negishi, Y. Tadano, M. Arifuku, N. Kiyoyanagi, T. Yamaguchi, K. Ishibashi and Y. Kobayashi
  • Organizer: 14th Int. Conf. on Atomically Controlled Surfaces, Interfaces and Nanostructures (ACSIN-14)
  • Int'l Joint Research
• [Presentation] Electrical transport properties of multilayer graphene nanoribbons (2018)
  • Author(s): R. Negishi, K. Yamamoto, M. Fukumori, T. Fujiwara, H. Tanaka and Y. Kobayashi
  • Organizer: 14th Int. Conf. on Atomically Controlled Surfaces, Interfaces and Nanostructures (ACSIN-14)
  • Int'l Joint Research
• [Presentation] Ultra-high Crystallinity Carbon Nanotube Grown from Carbon Nano-onion (2018)
  • Author(s): K. Nakamura, H. Semba, S.X. Li, M. Arifuku, N. Kiyoyanagi and Y. Kobayashi
  • Organizer: 14th Int. Conf. on Atomically Controlled Surfaces, Interfaces and Nanostructures (ACSIN-14)
  • Int'l Joint Research
• [Presentation] Turbostratic Multilayer Graphene Synthesis On CVD Graphene Template Toward Improving Electrical Performance (2018)
  • Author(s): C. Wei, R. Negishi, Y. Ogawa, M. Takamura, Y. Taniyasu and Y. Kobayashi
  • Organizer: 14th Int. Conf. on Atomically Controlled Surfaces, Interfaces and Nanostructures (ACSIN-14)
  • Int'l Joint Research
• [Presentation] グラフェンテンプレート上に成長した多層グラフェンの積層構造と電気伝導解析 (2018)
  • Author(s): 根岸 良太、魏 超鵬、姚 瑶、小川 友以、谷保 芳孝、小林 慶裕
  • Organizer: ２０１８年第79回応用物理学会秋季学術講演会
• [Presentation] グラフェン層成長における水添加効果 (2018)
  • Author(s): 根岸 良太、高村 真琴、谷保 芳孝、小林 慶裕
  • Organizer: ２０１８年第79回応用物理学会秋季学術講演会
• [Presentation] CVDグラフェンをテンプレートとしたグラフェン多層成長 (2018)
  • Author(s): 根岸 良太、丸岡 真人、小川 友以、高村 真琴、谷保 芳孝、小林 慶裕
  • Organizer: 第65回応用物理学会春季学術講演会
• [Presentation] 高温での機械剥離グラフェン上多層グラフェンの成長様式解析 (2018)
  • Author(s): 丸岡 真人、根岸 良太、小林 慶裕
  • Organizer: 第65回応用物理学会春季学術講演会
• [Presentation] 酸化グラフェン・セルロースナノファイバー複合体の超高温処理による高空隙ナノカーボン材料形成 (2018)
  • Author(s): 許 梓ショウ、中村 槙悟、仁科 勇太、小林 慶裕
  • Organizer: 第65回応用物理学会春季学術講演会
• [Presentation] ナノダイヤモンドからのCNT成長における同位体混合比制御 (2018)
  • Author(s): 大畑 惇貴、中村 圭介、有福 達治、清柳 典子、小林 慶裕
  • Organizer: 第65回応用物理学会春季学術講演会
• [Presentation] カーボンナノオニオンを核としたカーボンナノチューブの高温成長 (2018)
  • Author(s): 仙波 弘樹、有福 達治、清柳 典子、小林 慶裕
  • Organizer: 第65回応用物理学会春季学術講演会
• [Presentation] 超高温処理による酸化グラフェン構造修復過程の活性化エネルギー解析 (2018)
  • Author(s): 中村 槙悟、仁科 勇太、小林 慶裕
  • Organizer: 第65回応用物理学会春季学術講演会
• [Presentation] Band-like transport of highly crystalline graphene films from defective graphene oxides (2017)
  • Author(s): R. Negishi, and Y. Kobayashi
  • Organizer: Collaborative Conference on Material Research
  • Int'l Joint Research / Invited
• [Presentation] Investigation of surface potentials in reduced graphene oxide flake by Kelvin probe force microscopy (2017)
  • Author(s): R. Negishi, K. Takashima and Y. Kobayashi
  • Organizer: The 30th International Microprocesses and Nanotechnology Conference
  • Int'l Joint Research
• [Presentation] Improved electrical properties of reduced graphene oxide film by water-assisted thermal process (2017)
  • Author(s): R. Negishi, T. Nakagiri M. Akabori and Y. Kobayashi
  • Organizer: The 30th International Microprocesses and Nanotechnology Conference
  • Int'l Joint Research
• [Presentation] Band-like transport in highly crystalline graphene thin films from defective graphene oxide material (2017)
  • Author(s): R. Negishi, M. Akabori, T. Ito, Y. Watanabe, and Y. Kobayashi
  • Organizer: International Symposium on Hybrid Quantum Systems 2017 (HQS2017)
  • Int'l Joint Research
• [Presentation] Synthesis of turbostratic multilayer graphene film from graphene oxides by ultrahigh temperature process (2017)
  • Author(s): S. Nakamura, T. Ishida, Y. Nishina and Y. Kobayashi
  • Organizer: International Symposium on Hybrid Quantum Systems 2017 (HQS2017)
  • Int'l Joint Research
• [Presentation] Raman analysis on nanocarbon materials formation by isotope labelling toward 13C position control in graphitic lattice (2017)
  • Author(s): A. Ohata, X. Xizhao, T. Ishida and Y. Kobayashi
  • Organizer: International Symposium on Hybrid Quantum Systems 2017 (HQS2017)
  • Int'l Joint Research
• [Presentation] Scalable Synthesis of Turbostratic Multilayer Graphene Film from Graphene Oxides by Ultrahigh Temperature Process (2017)
  • Author(s): Yoshihiro Kobayashi, Shingo Nakamura, Takashi Ishida, Atsuki Ohata, Yuta Nishina
  • Organizer: 2017 MRS Fall Meeting
  • Int'l Joint Research
• [Presentation] 高温プロセスによる高結晶性多層グラフェンの成長 (2017)
  • Author(s): 根岸 良太、丸岡 真人、小林 慶裕
  • Organizer: 第78回応用物理学会秋季学術講演会
• [Presentation] ケルビンフォースプローブ顕微鏡による還元した酸化グラフェン薄膜の表面電位観察 (2017)
  • Author(s): 根岸 良太、高島 快、小林 慶裕
  • Organizer: 第78回応用物理学会秋季学術講演会
• [Presentation] カーボンナノオニオンを核としたカーボンナノチューブ成長 (2017)
  • Author(s): 仙波 弘樹、有福 達治、清柳 典子、小林 慶裕
  • Organizer: 第78回応用物理学会秋季講演会
• [Presentation] スポンジ状高空隙酸化グラフェンの超高温処理による乱層多層グラフェンの形成 (2017)
  • Author(s): 中村 槙悟、石田 俊、仁科 勇太、小林 慶裕
  • Organizer: 第78回応用物理学会秋季講演会
• [Remarks] ナノマテリアル領域ｗｅｂページ
  • URL: http://www.ap.eng.osaka-u.ac.jp/nanomaterial/index.html
• [Patent(Industrial Property Rights)] FIELD EFFECT TRANSISTOR AND SENSOR USING SAME (2017)
  • Inventor(s): Y. Kobayashi,N. Kiyoyanagi et al
  • Industrial Property Rights Holder: Y. Kobayashi,N. Kiyoyanagi et al
  • Industrial Property Rights Type: 特許
  • Filing Date: 2017
  • Overseas