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Rapid nucleation and crystallization induced by microsegregation of glasses

Research Project

Project/Area Number 19K15663
Research Category

Grant-in-Aid for Early-Career Scientists

Allocation TypeMulti-year Fund
Review Section Basic Section 36010:Inorganic compounds and inorganic materials chemistry-related
Research InstitutionNational Institute of Advanced Industrial Science and Technology

Principal Investigator

Shinozaki Kenji  国立研究開発法人産業技術総合研究所, 材料・化学領域, 主任研究員 (10723489)

Project Period (FY) 2019-04-01 – 2021-03-31
Project Status Completed (Fiscal Year 2020)
Budget Amount *help
¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2020: ¥1,560,000 (Direct Cost: ¥1,200,000、Indirect Cost: ¥360,000)
Fiscal Year 2019: ¥2,600,000 (Direct Cost: ¥2,000,000、Indirect Cost: ¥600,000)
Keywords核形成 / 不均質 / ナノ結晶 / 中距離構造 / X線全散乱 / 分子動力学法 / 第一原理計算 / アップコンバージョン / ガラス / 非晶質構造解析 / ミクロ偏析 / フッ化物ナノ結晶 / XAFS / 微小球 / 構造解析 / ゆらぎ / 太陽光波長変換材料 / 過冷却融液 / レーザー / 非晶質構造 / 結晶化
Outline of Research at the Start

ガラス中に機能性のナノ結晶を析出させることで、波長変換などの様々な機能性を持った機能性の高透明部材が得られる。ガラス(または過冷却融液)から析出する結晶の粒径は、核形成と結晶成長のそれぞれの速度の競合によって決まり、核形成が速く成長が遅ければ結晶粒径は小さくなる。本研究では、従来の長時間熱処理による結晶化とは一線を画す、融液冷却固化過程での超高速ナノ結晶化を目指す。ガラスの中距離構造、ミクロ偏析を設計することで、超高速の核形成が実現し、超短時間熱処理でナノ結晶化可能であることを実証するとともに、その材料設計指針を明らかにする。

Outline of Final Research Achievements

We proposed a new material design guideline for inducing microsegregation and enabled ultrafast nucleation via microsegregation as a nucleation site in this study. In order to investigate the structure of microsegregation, we analyzed the radial distribution function and performed molecular dynamics simulations. It was proposed that the mixing state of glass can be controlled by adding a third component of intermediate polarity to the fluorides such as BaF2 and oxides such as B2O3, which have low miscibility as suggested by the HBSA rule. This provides a guideline for designing a structure suitable for nucleation. Furthermore, we worked on the crystallization of glass during the cooling process of the melt, and demonstrated that nanocrystallization is possible during the cooling process.

Academic Significance and Societal Importance of the Research Achievements

ガラス(または過冷却融液)から析出する結晶の粒径は、核形成と結晶成長のそれぞれの速度の競合によって決まり、核形成が速く成長が遅ければ結晶粒径は小さくなる。結晶成長の制御は粘性の調整等の指針がある一方、核形成については十分理解が進んでおらず、これまでは試行錯誤により制御するしかなかった。本研究ではガラスと結晶の構造類似性の設計方法を提案し、ガラス構造設計により核形成を加速する指針を明らかにした。また、従来困難だった急冷過程でのナノ結晶化にも成功した。この成果はより高効率の材料開発及び、高生産性での材料作製やデバイス形成の実現につながる。

Report

(3 results)
  • 2020 Annual Research Report   Final Research Report ( PDF )
  • 2019 Research-status Report
  • Research Products

    (31 results)

All 2021 2020 2019 Other

All Int'l Joint Research (1 results) Journal Article (8 results) (of which Int'l Joint Research: 1 results,  Peer Reviewed: 6 results,  Open Access: 2 results) Presentation (21 results) (of which Int'l Joint Research: 11 results,  Invited: 3 results) Patent(Industrial Property Rights) (1 results)

  • [Int'l Joint Research] Coe College(米国)

    • Related Report
      2019 Research-status Report
  • [Journal Article] Up-conversion Luminescence Enhanced by the Plasmonic Lattice Resonating at the Transparent Window of Water2021

    • Author(s)
      Gao Yuan、Murai Shunsuke、Shinozaki Kenji、Tanaka Katsuhisa
    • Journal Title

      ACS Applied Energy Materials

      Volume: 4 Issue: 4 Pages: 2999-3007

    • DOI

      10.1021/acsaem.0c01826

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Photoluminescence and structural similarity of crystals with oxide–fluoride stacking structure and oxyfluoride glass2020

    • Author(s)
      SHINOZAKI Kenji、SUKENAGA Sohei、OHARA Koji
    • Journal Title

      Journal of the Ceramic Society of Japan

      Volume: 128 Issue: 12 Pages: 1030-1037

    • DOI

      10.2109/jcersj2.20168

    • NAID

      130007949055

    • ISSN
      1348-6535, 1882-0743
    • Year and Date
      2020-12-01
    • Related Report
      2020 Annual Research Report
  • [Journal Article] Impact of crystallization method on the strain, defect formation, and thermoluminescence of YAG: Ce crystals2020

    • Author(s)
      Kenji Shinozaki, Go Okada, Kiminori Sato, Ruize Yu, and Mario Affatigato
    • Journal Title

      Journal of Alloys and Compounds

      Volume: 849 Pages: 1566001-156606

    • DOI

      10.1016/j.jallcom.2020.156600

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Aluminum for Near Infrared Plasmonics: Amplified Up‐Conversion Photoluminescence from Core?Shell Nanoparticles on Periodic Lattices2020

    • Author(s)
      Gao Yuan、Murai Shunsuke、Shinozaki Kenji、Ishii Satoshi、Tanaka Katsuhisa
    • Journal Title

      Advanced Optical Materials

      Volume: 9 Issue: 1 Pages: 2001040-2001040

    • DOI

      10.1002/adom.202001040

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Structural origin of high-density Gd2O3-MoO3-B2O3 glass and low-density β'-Gd2(MoO4)3 crystal: a study conducted using high-energy x-ray diffraction and EXAFS at high temperatures2020

    • Author(s)
      Kenji Shinozaki, Hiroki Tsuchiya, Tsuyoshi Honma, Koji Ohara, Hirokazu Masai,Toshiaki Ina, Takayuki Komatsu
    • Journal Title

      Journal of Physics: Condensed Matter

      Volume: 32 Issue: 5 Pages: 055705-055705

    • DOI

      10.1088/1361-648x/ab4e64

    • Related Report
      2019 Research-status Report
    • Peer Reviewed
  • [Journal Article] Massive red shift of Ce3+ in Y3Al5O12 incorporating super-high content of Ce2020

    • Author(s)
      Nakamura Hitomi、Shinozaki Kenji、Okumura Toyoki、Nomura Katsuhiro、Akai Tomoko
    • Journal Title

      RSC Advances

      Volume: 10 Issue: 21 Pages: 12535-12546

    • DOI

      10.1039/d0ra01381a

    • Related Report
      2019 Research-status Report
    • Peer Reviewed
  • [Journal Article] Rapid Synthesis of Quantum-Sized Organic?Inorganic Perovskite Nanocrystals in Glass2020

    • Author(s)
      Shinozaki Kenji、Kawano Naoki
    • Journal Title

      Scientific Reports

      Volume: 10 Issue: 1 Pages: 1237-1237

    • DOI

      10.1038/s41598-020-58266-2

    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] 酸フッ化物ガラスの 構造と結晶化, 光機能2019

    • Author(s)
      篠崎健二
    • Journal Title

      セラミックス誌

      Volume: 54 Pages: 611-614

    • Related Report
      2019 Research-status Report
  • [Presentation] Photoluminescence and Scintillation in New Oxyfluoride Glasses with Designed Fluoride Segregation2020

    • Author(s)
      Kenji Shinozaki
    • Organizer
      Online Summit On Carbon materials and Nanotechnology
    • Related Report
      2020 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Glass structure of fluoroborate glasses precipitate NaYF4 nanocrystals and nanocrystallization in melt-quenching process2020

    • Author(s)
      Kenji Shinozaki, Koji Ohara
    • Organizer
      Glass Meeting 2020
    • Related Report
      2020 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Nanocrystallization of fluoroborate glasses and their structure, photoluminescence, and scintillation properties2020

    • Author(s)
      Kenji Shinozaki, Sohei Sukenaga, Koji Ohara, Noriaki Kawaguchi, Takayuki Yanagida
    • Organizer
      45th International Conference and Expo on Advanced Ceramics and Composites
    • Related Report
      2020 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] フツホウ酸ガラスの構造とNaYF4ナノ結晶化機構2020

    • Author(s)
      篠崎 健二、石井 良樹
    • Organizer
      The 31st Meeting on Glasses for Photonics
    • Related Report
      2020 Annual Research Report
  • [Presentation] Pr添加TeO2Al2O3BaOガラスの作製とシンチレーション特性評価2020

    • Author(s)
      高久 暁人、河野 直樹、木村 大海、中内 大介、赤塚 雅紀、篠崎 健二、柳田 健之
    • Organizer
      第81回応用物理学会秋季学術講演会
    • Related Report
      2020 Annual Research Report
  • [Presentation] 希土類モリブデン酸塩系ガラスが有する析出結晶よりも高い充填密度の構造的起源解明2020

    • Author(s)
      篠崎 健二、土屋 博樹、伊那 稔哲、尾原 幸治、本間 剛、小松 高行
    • Organizer
      日本セラミックス協会第33回秋季シンポジウム
    • Related Report
      2020 Annual Research Report
  • [Presentation] 酸フッ化物ガラスの冷却過程でのナノ結晶化ガラス微小球の作製とアップコンバージョン発光2020

    • Author(s)
      篠崎 健二、Gao Yuan、金高 健二、赤井 智子、岸 哲生、矢野 哲司
    • Organizer
      日本セラミックス協会第33回秋季シンポジウム
    • Related Report
      2020 Annual Research Report
  • [Presentation] Nanocrystallization of NaYF4 in fluoroborate glasses in melt-cooling process and the impact of glass structure2020

    • Author(s)
      Kenji Shinozaki
    • Organizer
      Virtual Glass Meeting 2020
    • Related Report
      2020 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Glass structure and nanocrystallization mechanism of BaF2-ZnO-B2O3 glasses2019

    • Author(s)
      Kenji Shinozaki, Yoshiki Ishii, Sohei Sukenaga, Hiroyuki Shibata, Koji Ohara
    • Organizer
      International Congress on Glass 2019
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] Impact of Additives on Nanocrystallization of BaF2 in Fluoroborate System2019

    • Author(s)
      Kenji Shinozaki
    • Organizer
      International Congress on Glass 2019
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] Photoluminescence and Scintillation in New Oxyfluoride Glasses with Designed Fluoride Segregation2019

    • Author(s)
      Kenji Shinozaki, Sohei Sukenaga, Hiroyuki Shibata, Koji Ohara, Go Okada, Noriaki Kawaguchi, Takayuki Yanagida
    • Organizer
      2nd Global Forum on Advanced Materials and Technologies for Sustainable Development (GFMAT-2)
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Synthesis, structure and physical properties of 1La2O3:2WO3:1B2O3 glass containing Nb2O52019

    • Author(s)
      Lyubomir I. Aleksandrov, Reni Iordanova, Margarita Milanova, Kenji Shinozaki, Takayuki Komatsu
    • Organizer
      International Congress on Glass 2019
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] Synthesis and Luminescence of Layered Organic-Inorganic Perovskite Nanocrystals in Glass2019

    • Author(s)
      Kenji Shinozaki, Naoki Kawano
    • Organizer
      2nd Global Forum on Advanced Materials and Technologies for Sustainable Development (GFMAT-2)
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] Nucleation mechanism from fluoride segregation in new transparent oxyfluoride crystallized glass2019

    • Author(s)
      Kenji Shinozaki, Sohei Sukenaga, Hiroyuki Shibata, Koji Ohara
    • Organizer
      2nd Global Forum on Advanced Materials and Technologies for Sustainable Development (GFMAT-2)
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] 希土類モリブデン酸塩系ガラスが有する析出結晶よりも高い充填密度の構造的起源解明 :高温XAFSおよび高温高エネルギーX線全散乱解析2019

    • Author(s)
      篠崎健二、土屋博樹、伊那稔哲、本間剛、小松高行
    • Organizer
      第60回ガラスおよびフォトニクス材料討論会
    • Related Report
      2019 Research-status Report
  • [Presentation] ガラス融液冷却過程でのBaF2ナノ結晶析出と中距離構造の効果2019

    • Author(s)
      篠崎健二、尾原幸治
    • Organizer
      The 30th Meeting on Glasses for Photonics
    • Related Report
      2019 Research-status Report
  • [Presentation] Ce3+ドープMgF2-Al2O3-B2O3ガラスの蛍光及びX線励起発光特性2019

    • Author(s)
      篠崎健二、中内大介、岡田豪、河口範明、柳田健之
    • Organizer
      第67回応用物理学会 春季学術講演会
    • Related Report
      2019 Research-status Report
  • [Presentation] 過冷却融液固化により合成したYAG:Ceの蛍光及び熱ルミネッセンス特性2019

    • Author(s)
      篠崎健二、岡田豪、Mario Affatigato
    • Organizer
      第67回応用物理学会 春季学術講演会
    • Related Report
      2019 Research-status Report
  • [Presentation] 融液急冷過程でフッ化物ナノ結晶析出させた透明結晶化ガラスファイバー及び微小球作製2019

    • Author(s)
      篠崎健二、赤井智子、岸哲生、矢野哲司
    • Organizer
      日本セラミックス協会2020年年会
    • Related Report
      2019 Research-status Report
  • [Presentation] ハロゲン含有ガラスの融液冷却過程での透明ナノ結晶化2019

    • Author(s)
      篠崎健二、尾原幸治、赤井智子
    • Organizer
      第60回ガラスおよびフォトニクス材料討論会
    • Related Report
      2019 Research-status Report
  • [Presentation] The Structural Origin of High Density of Gd2O3-MoO3-B2O3 Glass and Low Density of b"-Gd2(MoO4)3 Crystal Investigated by High-Energy X-ray Diffraction at High Temperature2019

    • Author(s)
      Kenji Shinozaki, Hiroki Tsuchiya, Tsuyoshi Honma, Koji Ohara, Hirokazu Masai, Toshiaki Ina, Takayuki Komatsu
    • Organizer
      The 13th Pacific Rim Conference of Ceramic Societies
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Patent(Industrial Property Rights)] 結晶化ガラスおよびその製造方法2020

    • Inventor(s)
      篠崎健二、赤井智子
    • Industrial Property Rights Holder
      国立研究開発法人産業技術総合研究所
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      2018-113179
    • Filing Date
      2020
    • Related Report
      2019 Research-status Report

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Published: 2019-04-18   Modified: 2022-01-27  

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