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Synthesis of high quality single crystals for sience of Boron Nitride

Research Project

Project/Area Number 20H00354
Research Category

Grant-in-Aid for Scientific Research (A)

Allocation TypeSingle-year Grants
Section一般
Review Section Medium-sized Section 30:Applied physics and engineering and related fields
Research InstitutionNational Institute for Materials Science

Principal Investigator

TANIGUCHI Takashi  国立研究開発法人物質・材料研究機構, 国際ナノアーキテクトニクス研究拠点, 拠点長 (80354413)

Co-Investigator(Kenkyū-buntansha) 町田 友樹  東京大学, 生産技術研究所, 教授 (00376633)
山田 貴壽  国立研究開発法人産業技術総合研究所, 材料・化学領域, 研究チーム長 (30306500)
小島 一信  大阪大学, 大学院工学研究科, 教授 (30534250)
宮川 仁  国立研究開発法人物質・材料研究機構, 機能性材料研究拠点, 主任研究員 (40552667)
秩父 重英  東北大学, 多元物質科学研究所, 教授 (80266907)
Project Period (FY) 2020-04-01 – 2023-03-31
Project Status Completed (Fiscal Year 2022)
Budget Amount *help
¥45,240,000 (Direct Cost: ¥34,800,000、Indirect Cost: ¥10,440,000)
Fiscal Year 2022: ¥12,480,000 (Direct Cost: ¥9,600,000、Indirect Cost: ¥2,880,000)
Fiscal Year 2021: ¥17,290,000 (Direct Cost: ¥13,300,000、Indirect Cost: ¥3,990,000)
Fiscal Year 2020: ¥15,470,000 (Direct Cost: ¥11,900,000、Indirect Cost: ¥3,570,000)
Keywords六方晶窒化ホウ素 / 高圧合成 / 遠紫外線発光 / 反応性溶媒 / 高純度単結晶 / 2次元光・電子デバイス / インターカーレーション / 六方晶窒化ホウ素単結晶 / 合成合成 / 不純物制御 / 窒化ホウ素 / 高圧下結晶成長 / 2次元原子層基板
Outline of Research at the Start

窒化ホウ素(BN)は炭素と類似の結晶構造を有し、黒鉛型の六方晶(hBN)は耐熱材料、絶縁材料等として産業応用されている。このhBNの応用は炭素材料の多様性と比較して未だ限定的と云えるが、近年新たな半導体材料としての展開が進みつつある。本課題では現行の不純物がppmにとどまっている高純度化のレベルをppb領域にまで引き上げた高品位化を実現し、hBNの遠紫外線発光素子の高効率化を始めとしたBNの科学の基礎を先導する。更に、hBNへの半導体化は最大の課題であるが、高純度単結晶を獲得した上で、適切なドーピングと半導体特性の評価、制御に挑戦する。

Outline of Final Research Achievements

We optimized the crystal growth solvent and obtained high-quality hexagonal boron nitride (hBN) single crystals with a residual carbon impurity concentration of several 10 ppb level (EPR evaluation) under high pressure. There is a strong correlation between the far-ultraviolet luminescence efficiency of the high-purity crystal and the amount of residual carbon impurities, and we obtained a rough estimate of the external quantum efficiency of the high-quality crystal of about 3%. It was found that although hBN is an indirect transition emiconductor, it is easy to emit light due to the presence of many phonons that match the momentum change required for luminescence and the existence of a flat energy band region. Furthermore, K-doped hBN was obtained using an aqueous potassium hydroxide solution by an electrochemical method. In addition, collaboration with domestic and foreign institutions as an insulating substrate for two-dimensional atomic layer devices was also promoted.

Academic Significance and Societal Importance of the Research Achievements

窒化ホウ素(BN)は炭素と類似の結晶構造を有し、黒鉛型の六方晶(hBN)は耐熱材料、絶縁材料等として産業応用されている。本研究では高純度化のレベルをppb領域にまで引き上げたhBN結晶の高品位化とその遠紫外線発光素子の高効率化を見いだした。hBNへのドー ピングによる半導体化は最大の課題であるが、電気化学的手法による水酸化カリウム水溶液を用いて、K添加hBNの合成に成功した。半導体特性評価のため、電界効果トランジスタ構造によるよる評価手法の確立が課題である。本課題により、2次元原子層デバイス基盤としての活用も含め、hBNの新たな半導体材料として基礎の確立に向けた成果を得ることが出来た。

Report

(5 results)
  • 2022 Annual Research Report   Final Research Report ( PDF )
  • 2021 Annual Research Report
  • 2020 Comments on the Screening Results   Annual Research Report
  • Research Products

    (44 results)

All 2023 2022 2021 2020 Other

All Int'l Joint Research (9 results) Journal Article (21 results) (of which Int'l Joint Research: 16 results,  Peer Reviewed: 21 results,  Open Access: 3 results) Presentation (13 results) (of which Int'l Joint Research: 9 results,  Invited: 11 results) Patent(Industrial Property Rights) (1 results)

  • [Int'l Joint Research] コロンビア大学/ハーバード大学/ワシントン大学(米国)

    • Related Report
      2022 Annual Research Report
  • [Int'l Joint Research] ドルトムント大/ミュンヘン工科大/レーゲンスブルグ大(ドイツ)

    • Related Report
      2022 Annual Research Report
  • [Int'l Joint Research] MIT/Columbia Univ/Harvard Univ.(米国)

    • Related Report
      2021 Annual Research Report
  • [Int'l Joint Research] Univ.Suttutgard(ドイツ)

    • Related Report
      2021 Annual Research Report
  • [Int'l Joint Research] MIT/ハーバード大/UCバークレー(米国)

    • Related Report
      2020 Annual Research Report
  • [Int'l Joint Research] SNU/NTU(シンガポール)

    • Related Report
      2020 Annual Research Report
  • [Int'l Joint Research] CNRS(フランス)

    • Related Report
      2020 Annual Research Report
  • [Int'l Joint Research] ICFO(スペイン)

    • Related Report
      2020 Annual Research Report
  • [Int'l Joint Research] フダン大/南京大/北京大(中国)

    • Related Report
      2020 Annual Research Report
  • [Journal Article] Evidence for unconventional superconductivity in twisted trilayer graphene2022

    • Author(s)
      Kim Hyunjin、Choi Youngjoon、Lewandowski Cyprian、Thomson Alex、Zhang Yiran、Polski Robert、Watanabe Kenji、Taniguchi Takashi、Alicea Jason、Nadj-Perge Stevan
    • Journal Title

      Nature

      Volume: 606 Issue: 7914 Pages: 494-500

    • DOI

      10.1038/s41586-022-04715-z

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Steep-slope Schottky diode with cold metal source2022

    • Author(s)
      Shin Wongil、Myeong Gyuho、Sung Kyunghwan、Kim Seungho、Lim Hongsik、Kim Boram、Jin Taehyeok、Park Jihoon、Watanabe Kenji、Taniguchi Takashi、Liu Fei、Cho Sungjae
    • Journal Title

      Applied Physics Letters

      Volume: 120 Issue: 24 Pages: 243506-243506

    • DOI

      10.1063/5.0097408

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Tuning colour centres at a twisted hexagonal boron nitride interface2022

    • Author(s)
      Su Cong、Zhang Fang、Kahn Salman、Shevitski Brian、Jiang Jingwei、Dai Chunhui、Ungar Alex、Park Ji-Hoon、Watanabe Kenji、Taniguchi Takashi、Kong Jing、Tang Zikang、Zhang Wenqing、Wang Feng、Crommie Michael、Louie Steven G.、Aloni Shaul、Zettl Alex
    • Journal Title

      Nature Materials

      Volume: 21 Issue: 8 Pages: 896-902

    • DOI

      10.1038/s41563-022-01303-4

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Current Injection into Single-Crystalline Carbon-Dope h-BN toward Electronic and Optoelectronic Applications2022

    • Author(s)
      Ngamprapawat Supawan、Nishimura Tomonori、Watanabe Kenji、Taniguchi Takashi、Nagashio Kosuke
    • Journal Title

      ACS Applied Materials and Interfaces

      Volume: 14 Issue: 22 Pages: 25731-25740

    • DOI

      10.1021/acsami.2c04544

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Electrically tunable quantum confinement of neutral excitons2022

    • Author(s)
      Thureja Deepankur、Imamoglu Atac、Smoleski Tomasz、Amelio Ivan、Popert Alexander、Chervy Thibault、Lu Xiaobo、Liu Song、Barmak Katayun、Watanabe Kenji、Taniguchi Takashi、Norris David J.、Kroner Martin、Murthy Puneet A.
    • Journal Title

      Nature

      Volume: 606 Issue: 7913 Pages: 298-304

    • DOI

      10.1038/s41586-022-04634-z

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Ultrafast Operation of 2D Heterostructured Nonvolatile Memory Devices Provided by the Strong Short-Time Dielectric Breakdown Strength of h-BN2022

    • Author(s)
      T. Sasaki, K. Ueno, T. Taniguchi, K. Watanabe, T. Nishimura, and K. Nagashio
    • Journal Title

      ACS Appl. Mater. Interfaces

      Volume: 14 Issue: 22 Pages: 25659-25669

    • DOI

      10.1021/acsami.2c03198

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Odd-even Layer-number Effect of Valence-band Spin Splitting in WTe22022

    • Author(s)
      M. Sakano, Y. Tanaka, S. Masubuchi, S. Okazaki, T. Nomoto, A. Oshima, K. Watanabe, T. Taniguchi, R. Arita, T. Sasagawa, T. Machida, and K. Ishizaka
    • Journal Title

      Phys. Rev. Research

      Volume: 4 Issue: 2 Pages: 023247-023247

    • DOI

      10.1103/physrevresearch.4.023247

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Subband-resolved momentum-conserved resonant tunneling in monolayer graphene/h-BN/ABA-trilayer graphene small-twist-angle tunneling device2022

    • Author(s)
      Seo Yuta、Masubuchi Satoru、Onodera Momoko、Zhang Yijin、Moriya Rai、Watanabe Kenji、Taniguchi Takashi、Machida Tomoki
    • Journal Title

      Applied Physics Letters

      Volume: 120 Issue: 8 Pages: 083102-083102

    • DOI

      10.1063/5.0080215

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Quantum anomalous Hall effect from intertwined moire bands2021

    • Author(s)
      Tingxin Li, Shengwei Jiang, Bowen Shen, Yang Zhang, Lizhong Li, Zui Tao, Trithep Devakul, Kenji Watanabe, Takashi Taniguchi, Liang Fu, Jie Shan, Kin Fai Mak.
    • Journal Title

      Nature

      Volume: 600 Issue: 7890 Pages: 641-646

    • DOI

      10.1038/s41586-021-04171-1

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Evidence for unconventional superconductivity in twisted bilayer graphene.2021

    • Author(s)
      Myungchul Oh, Kevin P. Nuckolls, Dillon Wong, Ryan L. Lee, Xiaomeng Liu, Kenji Watanabe, Takashi Taniguchi, Ali Yazdani.
    • Journal Title

      Nature

      Volume: 600 Issue: 7888 Pages: 240-245

    • DOI

      10.1038/s41586-021-04121-x

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Direct visualization of magnetic domains and moire magnetism in twisted 2D magnets.2021

    • Author(s)
      Tiancheng Song, Qi-Chao Sun, Eric Anderson, Chong Wang, Jimin Qian, Takashi Taniguchi, Kenji Watanabe, Michael A. McGuire, Rainer Stehr, Di Xiao, Ting Cao, Jorg Wrachtrup, Xiaodong Xu
    • Journal Title

      Science

      Volume: 374 Issue: 6571 Pages: 1140-1144

    • DOI

      10.1126/science.abj7478

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Quantum criticality in twisted transition metal dichalcogenides.2021

    • Author(s)
      Augusto Ghiotto, En-Min Shih, Giancarlo S. S. G. Pereira, Daniel A. Rhodes, Bumho Kim, Jiawei Zang, Andrew J. Millis, Kenji Watanabe, Takashi Taniguchi, James C. Hone, Lei Wang, Cory R. Dean, Abhay N. Pasupathy.
    • Journal Title

      Nature

      Volume: 597 Issue: 7876 Pages: 345-349

    • DOI

      10.1038/s41586-021-03815-6

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Temperature dependence of carrier mobility in chemical vapor deposited graphene on high-pressure, high-temperature hexagonal boron nitride2021

    • Author(s)
      Yuki Okigawa, Tomoaki Masuzawa, Kenji Watanabe, Takashi Taniguchi, Takatoshi Yamada
    • Journal Title

      Applied Surface Science

      Volume: 562 Pages: 150146-150146

    • DOI

      10.1016/j.apsusc.2021.150146

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 2D-3D integration of hexagonal boron nitride and a high-κ dielectric for ultrafast graphene-based electro-absorption modulators2021

    • Author(s)
      H. Agarwal, B. Terres, L. Orsini, A. Montanaro, V. Sorianello, M. Pantouvaki, K. Watanabe, T. Taniguchi, D. V. Thourhout, M. Romagnoli, and F. H. L. Koppens
    • Journal Title

      Nat. Commun.

      Volume: 12 Issue: 1 Pages: 1070-1704

    • DOI

      10.1038/s41467-021-20926-w

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Unconventional ferroelectricity in moire heterostructures2020

    • Author(s)
      Z. Zheng, Q. Ma, Z. Bi, S. de la Barrera, M.-H. Liu, N. Mao, Y. Zhang, N. Kiper, K. Watanabe, T. Taniguchi, J. Kong, W. A. Tisdale, R. Ashoori, N. Gedik, L. Fu, S.-Y. Xu, and P. Jarillo-Herrero
    • Journal Title

      Nature

      Volume: 588 Issue: 7836 Pages: 71-76

    • DOI

      10.1038/s41586-020-2970-9

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Circular electromechanical resonators based on hexagonal-boron nitride-graphene heterostructures2020

    • Author(s)
      R. Kumar, D. W. Session, R. Tsuchikawa, M. Homer, H. Paas, K. Watanabe, T. Taniguchi, and V. V. Deshpande
    • Journal Title

      Appl. Phys. Lett.

      Volume: 117 Issue: 18 Pages: 183103-4

    • DOI

      10.1063/5.0024583

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Relationship between mobility and strain in CVD graphene on h-BN2020

    • Author(s)
      T. Yamada, Y. Okigawa, M. Hasegawa, K. Watanabe, and T. Taniguchi
    • Journal Title

      AIP Adv.

      Volume: 10 Issue: 8 Pages: 085309-4

    • DOI

      10.1063/5.0019621

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Long lifetime of the E1u in-plane infrared-active modes of h-BN2020

    • Author(s)
      A. Segura, R. Cusce, T. Taniguchi, K. Watanabe, and L. Arts
    • Journal Title

      Phys. Rev. B

      Volume: 101 Issue: 23 Pages: 235203-4

    • DOI

      10.1103/physrevb.101.235203

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Hexagonal Boron Nitride As an Ideal Substrate for Carbon Nanotube Photonics2020

    • Author(s)
      N. Fang, K. Otsuka, A. Ishii, T. Taniguchi, K. Watanabe, K. Nagashio, and Y. K. Kato
    • Journal Title

      ACS Photonics

      Volume: 7 Issue: 7 Pages: 1773-1779

    • DOI

      10.1021/acsphotonics.0c00406

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Midgap radiative centers in carbon-enriched hexagonal boron2020

    • Author(s)
      M. Koperski, D. Vaclavkova, K. Watanabe, T. Taniguchi, K. Novoselov, M.
    • Journal Title

      Proc. Natl. Acad. Sci. U.S.A.

      Volume: 117 Issue: 24 Pages: 13214-13214

    • DOI

      10.1073/pnas.2003895117

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] High-Q dark hyperbolic phonon-polaritons in hexagonal boron nitride nanostructures2020

    • Author(s)
      G. Ramer, M. Tuteja, J. R. Matson, M. Davanco, T. G. Folland, A. Kretinin, T. Taniguchi, K. Watanabe, K. S. Novoselov, J. D. Caldwell, and A. Centrone
    • Journal Title

      Nanophotonics

      Volume: 9 Issue: 6 Pages: 1457-1467

    • DOI

      10.1515/nanoph-2020-0048

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Presentation] Synthesis of boron nitride single crystals under high pressure and impurity/isotope control for their functionalization2023

    • Author(s)
      T.Taniguchi
    • Organizer
      APS March meeting 2023
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Impurity and isotope control of Boron Nitride crystals and their properties2022

    • Author(s)
      T.Taniguchi
    • Organizer
      21th International Symposium on Boron, Borides, and Related Materials
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 六方晶窒化ホウ素のバルク結晶成長2022

    • Author(s)
      谷口 尚
    • Organizer
      2022年第83回応用物理学会秋季学術講演会
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Impurity control for diamond and boron nitride single crystals growth under high pressure2022

    • Author(s)
      T.Taniguchi
    • Organizer
      15th International Conference on New Diamond and Nano Carbon 2022
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] High pressure synthesis of hBN and other 2D single crystals2022

    • Author(s)
      T.Taniguchi
    • Organizer
      KPS-JSAP ジョイントシンポジウム The future of van der Waals structures
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Thickness dependence of h-BN on electrical properties of CVD graphene2022

    • Author(s)
      Takatoshi Yamada、Yuki Okigawa, Takashi Taniguchi
    • Organizer
      15th International Conference on New Diamond and Nano Carbon 2022
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] CVDグラフェンの電気特性のh-BN膜厚依存性2022

    • Author(s)
      山田 貴壽、沖川 侑揮、増澤 智昭、小川修一、谷口尚
    • Organizer
      第83回応用物理学会秋春季学術講演会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Solution growth of boron nitride single crystals under high pressure and their defect characterizations2021

    • Author(s)
      T. Taniguchi
    • Organizer
      the 12th International Conference on Advanced Materials and Devices (ICAMD 2021)
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] ”High Pressure Synthesis of Boron Nitride Crystals by Using a Reactive Solvent2021

    • Author(s)
      T. Taniguchi
    • Organizer
      the 10th Asian Conference on High Pressure Research
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Impurity control of Hexagonal Boron Nitride Crystals by flux growth process2021

    • Author(s)
      T.Taniguchi
    • Organizer
      34th International Microprocesses and Nanotechnology Conference(MNC2021)
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] Single Crystalline Hexagonal Boron Nitride for 2D Opto-Electric Devices2021

    • Author(s)
      T.Taniguchi
    • Organizer
      49th International Conference on the Physics of Semiconductors , Jaszowiec2021
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Synthesis of BN crystals by using solvent growth and their defect characterization2021

    • Author(s)
      T.Taniguchi
    • Organizer
      ACCGE-22/OMVPE-20:
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] Boron Nitride single crystals as wide band gap materials2021

    • Author(s)
      T.Taniguchi
    • Organizer
      NDNC2020/2021
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Patent(Industrial Property Rights)] 金属イオンでドープされた六方晶窒化ホウ素膜とその作製方法2023

    • Inventor(s)
      山田貴壽、谷口尚
    • Industrial Property Rights Holder
      山田貴壽、谷口尚
    • Industrial Property Rights Type
      特許
    • Filing Date
      2023
    • Related Report
      2022 Annual Research Report

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Published: 2020-04-28   Modified: 2024-01-30  

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