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Development of high-efficiency photoluminescent silica glasses of dense aggregates of photoactive centers

Research Project

Project/Area Number 19H02802
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 36010:Inorganic compounds and inorganic materials chemistry-related
Research InstitutionTokyo Metropolitan University

Principal Investigator

Kajihara Koichi  東京都立大学, 都市環境科学研究科, 教授 (90293927)

Project Period (FY) 2019-04-01 – 2023-03-31
Project Status Completed (Fiscal Year 2022)
Budget Amount *help
¥16,770,000 (Direct Cost: ¥12,900,000、Indirect Cost: ¥3,870,000)
Fiscal Year 2022: ¥2,340,000 (Direct Cost: ¥1,800,000、Indirect Cost: ¥540,000)
Fiscal Year 2021: ¥4,290,000 (Direct Cost: ¥3,300,000、Indirect Cost: ¥990,000)
Fiscal Year 2020: ¥3,900,000 (Direct Cost: ¥3,000,000、Indirect Cost: ¥900,000)
Fiscal Year 2019: ¥6,240,000 (Direct Cost: ¥4,800,000、Indirect Cost: ¥1,440,000)
Keywordsシリカガラス / 光活性中心凝集体 / 希土類イオン / エネルギー移動 / ナノ結晶 / シリカ
Outline of Research at the Start

一般に、発光中心は凝集すると発光効率が著しく低下する。この現象は「濃度消光」として知られており、多くの固体発光材料で、発光中心の高濃度化を阻んできた。しかし、凝集体がナノサイズで消光中心をほとんど含まない場合、濃度消光と、凝集体のレイリー散乱による透過損失が、ともに解消できる可能性がある。
本研究は、優れた透明性、強い光・放射線・化学腐食に対する耐久性を兼備したシリカガラス中に希土類イオンなどの発光性光活性中心の高濃度ナノ凝集体を形成することで、高効率発光と近接した光活性中心間での高効率エネルギー移動を両立させるもので、過酷環境下やエネルギー変換で使用できる堅牢な発光材料の実現を目指す。

Outline of Final Research Achievements

The aggregation of photoactive centers like rare-earth ions usually leads to a decrease in emission efficiency. This phenomenon is commonly known as "concentration quenching," and prevents to increase the concentration of photoactive centers in many solid-state phosphors. On the other hand, if quenching centers are absent, emission quenching may not occur even in the dense aggregates of photoactive centers. Based on this idea, silica glasses containing dense aggregates of rare-earth ions were employed in developing high-efficiency phosphors that utilize energy transfer. Silica-REPO4 transparent glass-ceramics that contain nanocrystals of rare-earth orthophosphates with diameters of ~5-10 nm provided unique opportunities to realize concentration-quenching-free visible or ultraviolet phosphors with internal quantum efficiencies close to unity, in which free energy migration and high efficiency emission coexist.

Academic Significance and Societal Importance of the Research Achievements

「濃度消光」という表現は学術用語として広く使われており、光活性中心が凝集すると必ず発光効率が下がるような印象を与えている。これに対し、本研究では、「濃度」と「消光」は必然関係にはなく、消光中心をなくすことで濃度消光を回避できる場合があることを実証した。シリカガラスは優れた透明性、強い光・放射線・化学腐食に対する耐久性、光ファイバーなどへの自由な成形性を兼備したガラスであることから、本研究で得られた知見は特に過酷環境下やエネルギー変換で使用できる堅牢な高効率透明発光材料の開発に有用であると期待される。

Report

(5 results)
  • 2022 Annual Research Report   Final Research Report ( PDF )
  • 2021 Annual Research Report
  • 2020 Annual Research Report
  • 2019 Annual Research Report
  • Research Products

    (29 results)

All 2023 2022 2021 2020 2019 Other

All Journal Article (6 results) (of which Peer Reviewed: 5 results,  Open Access: 2 results) Presentation (21 results) (of which Int'l Joint Research: 6 results,  Invited: 6 results) Book (1 results) Remarks (1 results)

  • [Journal Article] ゾル-ゲル法によるシリカ-REPO4透明結晶化ガラスの無濃度消光緑色・紫外発光2023

    • Author(s)
      梶原浩一
    • Journal Title

      NEW GLASS

      Volume: 37

    • Related Report
      2022 Annual Research Report
  • [Journal Article] Current status of sol–gel processing of glasses, ceramics, and organic–inorganic hybrids: a brief review2022

    • Author(s)
      Kajihara Koichi、Kanamori Kazuyoshi、Shimojima Atsushi
    • Journal Title

      Journal of the Ceramic Society of Japan

      Volume: 130 Issue: 8 Pages: 575-583

    • DOI

      10.2109/jcersj2.22078

    • ISSN
      1348-6535, 1882-0743
    • Year and Date
      2022-08-01
    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Cosolvent-free synthesis of macroporous silica gels and monolithic silica glasses from tetraalkoxysilane-water binary systems: comparison between tetramethoxysilane and tetraethoxysilane2022

    • Author(s)
      Kajihara Koichi、Goto Mioko
    • Journal Title

      Journal of Sol-Gel Science and Technology

      Volume: 104 Issue: 3 Pages: 497-502

    • DOI

      10.1007/s10971-022-05799-9

    • Related Report
      2022 Annual Research Report 2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Energy transfer and quenching in sol-gel-derived silica glass green phosphors doped with Tb3+ and Ce3+ ions: Distinct difference between P- and Al-codoped glasses2022

    • Author(s)
      K. Kajihara, S. Nakagawa, R. Iwasaki
    • Journal Title

      Phys. Status Solidi

      Volume: 219 Issue: 2 Pages: 2100494-2100494

    • DOI

      10.1002/pssa.202100494

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Negligible concentration quenching in photoluminescent nanocrystals with high photoactive rare-earth concentrations: silica?(Tb,Ce)PO4 transparent glass-ceramic green phosphors2021

    • Author(s)
      Iwasaki Rena、Kajihara Koichi
    • Journal Title

      Journal of Materials Chemistry C

      Volume: 9 Issue: 8 Pages: 2701-2705

    • DOI

      10.1039/d0tc06043g

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Cosolvent-free sol–gel dip-coating of silica films from tetraalkoxysilane–water binary systems: precursor solutions of long pot life and their characterization by nuclear magnetic resonance spectroscopy2020

    • Author(s)
      KAJIHARA Koichi、HIRUTA Keiichi、KANAMURA Kiyoshi
    • Journal Title

      Journal of the Ceramic Society of Japan

      Volume: 128 Issue: 10 Pages: 772-782

    • DOI

      10.2109/jcersj2.20150

    • NAID

      130007921314

    • ISSN
      1348-6535, 1882-0743
    • Year and Date
      2020-10-01
    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Presentation] シリカ-希土類リン酸塩透明結晶化ガラスの液相合成と無濃度消光緑色・紫外発光2023

    • Author(s)
      梶原 浩一
    • Organizer
      日本材料学会ナノ材料部門委員会 2022年度第2回研究会(京都大学桂キャンパス)
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] ゾル-ゲル法によるガラス合成2023

    • Author(s)
      梶原 浩一
    • Organizer
      日本セラミックス協会2023年年会基礎セミナー(神奈川大学みなとみらいキャンパス+オンライン)
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] TMOS-TEOS 混合溶液からの多孔質シリカゲルの無共溶媒ゾル-ゲル合成2023

    • Author(s)
      是枝 洸佳、石島 政直、梶原 浩一
    • Organizer
      日本セラミックス協会2023年年会(神奈川大学みなとみらいキャンパス+オンライン)
    • Related Report
      2022 Annual Research Report
  • [Presentation] 無共溶媒ゾル-ゲル法によるシリカ-(M,Ce)PO4(M = La, Y, Lu)透明結晶化ガラスの合成と発光特性2023

    • Author(s)
      高須 圭祐、石島 政直、梶原 浩一
    • Organizer
      日本セラミックス協会2023年年会(神奈川大学みなとみらいキャンパス+オンライン)
    • Related Report
      2022 Annual Research Report
  • [Presentation] Temperature dependence of narrow-band UVB photoluminescence of silica-(Gd,Pr)PO4 transparent glass-ceramics2023

    • Author(s)
      Koichi Kajihara, Shingo Nakagawa, Masanao Ishijima
    • Organizer
      The 14th international conference on SiO2, advanced dielectrics and related devices (SiO2 2023, Palermo, Italy)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] ゾル-ゲル法を用いた機能性ガラス合成2022

    • Author(s)
      梶原 浩一
    • Organizer
      日本ゾル-ゲル学会第19回セミナー(オンライン)
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] シリカ-希土類リン酸塩透明結晶化ガラスの無濃度消光緑色・紫外発光2022

    • Author(s)
      梶原 浩一
    • Organizer
      2022年度東京工業大学フロンティア材料研究所 先端無機材料共同研究拠点成果報告会(オンライン)
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] 四官能ケイ素アルコキシド-水二成分系からのマクロ多孔質シリカゲルとシリカガラスの無共溶媒合成2022

    • Author(s)
      梶原 浩一、後藤 美桜子
    • Organizer
      第83回応用物理学会秋季学術講演会(東北大学川内北キャンパス+オンライン)
    • Related Report
      2022 Annual Research Report
  • [Presentation] シリカ-(Gd,Pr)PO4 透明結晶化ガラスの狭帯域 UVB 発光の温度依存性2022

    • Author(s)
      中川 慎牙,石島 政直,梶原 浩一
    • Organizer
      第83回応用物理学会秋季学術講演会(東北大学川内北キャンパス+オンライン)
    • Related Report
      2022 Annual Research Report
  • [Presentation] ゾル-ゲル法によるシリカ-EuPO4透明結晶化ガラスの赤色発光2022

    • Author(s)
      眞田理子、梶原浩一
    • Organizer
      日本セラミックス協会2022年年会(オンライン・東京理科大学葛飾キャンパス)
    • Related Report
      2021 Annual Research Report
  • [Presentation] Negligible concentration quenching in sol-gel-derived silica-(Tb,Ce)PO4 transparent glass-ceramic green phosphors2021

    • Author(s)
      K. Kajihara, R. Iwasaki
    • Organizer
      13th International Symposium on SiO2, Advanced Dielectrics and Related Devices (Online/Lille, France)
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Tb,Ceドープシリカガラスの発光とエネルギ移動に共添加元素が及ぼす影響: PとAlの相違2021

    • Author(s)
      中川慎冴、岩﨑 玲奈、梶原浩一
    • Organizer
      日本セラミックス協会 第34回秋季シンポジウム(オンライン・山梨大学)
    • Related Report
      2021 Annual Research Report
  • [Presentation] シリカ-(Tb,Ce)PO4透明結晶化ガラスにおける無濃度消光緑色発光と高効率エネルギー移動2021

    • Author(s)
      梶原 浩一、岩﨑 玲奈
    • Organizer
      第62回ガラスおよびフォトニクス材料討論会(オンライン)
    • Related Report
      2021 Annual Research Report
  • [Presentation] シリカ系材料の無共溶媒ゾル-ゲル合成2021

    • Author(s)
      梶原浩一
    • Organizer
      高分子学会 第40回無機高分子研究討論会(オンライン)
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] Acid-catalyzed tetraalkoxysilane-water binary solutions: liquid-state NMR characterization and silica thin film processing2021

    • Author(s)
      K. Kajihara, K. Hiruta, K. Kanamura
    • Organizer
      14th Pacific Rim Conference on Ceramic and Glass Technology (PACRIM 14) (Online/Vancouver, Canada)
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 無共溶媒ゾル-ゲル法による長可使時間シリカ成膜溶液の液体NMR による評価2021

    • Author(s)
      梶原浩一、蛭田圭一、金村聖志
    • Organizer
      日本セラミックス協会2021年年会
    • Related Report
      2020 Annual Research Report
  • [Presentation] エステル交換によるゾル-ゲル法合成したシリカガラスのSiOH基濃度低減2021

    • Author(s)
      後藤美桜子、梶原浩一
    • Organizer
      日本セラミックス協会2021年年会
    • Related Report
      2020 Annual Research Report
  • [Presentation] シリカ-(Tb,Ce)PO4透明結晶化ガラスにおける無濃度消光緑色発光2020

    • Author(s)
      岩﨑玲奈、梶原浩一
    • Organizer
      第68回応用物理学会春季学術講演会
    • Related Report
      2020 Annual Research Report
  • [Presentation] Highly-transparent efficient sol-gel-derived silica-(Gd,Pr)PO4 glass-ceramic narrow-band UVB phosphors2019

    • Author(s)
      K. Kajihara, M. Suda, R. Nakagawa, K. Kajihara
    • Organizer
      The 8th International Workshop on Photoluminescence in Rare Earths: Photonic Materials and Devices (PRE19), Nice, France
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Photoluminescence of sol-gel-derived transparent silica-(Tb,Ce)PO4 glass- ceramics2019

    • Author(s)
      R. Iwasaki, K. Kajihara
    • Organizer
      The 13th Pacific Rim Conference of Ceramic Societies (PACRIM13), Okinawa, Japan
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Photoluminescence of sol-gel-derived transparent silica-(Gd,Pr)PO4 glass-ceramics under excitation with a KrCl excimer lamp2019

    • Author(s)
      R. Nakagawa, K. Kajihara
    • Organizer
      The 13th Pacific Rim Conference of Ceramic Societies (PACRIM13), Okinawa, Japan
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Book] ゾル-ゲル法技術の最新動向, 中西和樹(編)2023

    • Author(s)
      梶原浩一
    • Publisher
      シーエムシー出版
    • Related Report
      2022 Annual Research Report
  • [Remarks] 梶原研究室ホームページ

    • URL

      https://www.comp.tmu.ac.jp/kajiharalab/

    • Related Report
      2022 Annual Research Report 2021 Annual Research Report 2020 Annual Research Report 2019 Annual Research Report

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Published: 2019-04-18   Modified: 2024-01-30  

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