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Super-resolution fluorescence lifetime imaging microscopy using photon-photon and electron-photon correlations

Research Project

Project/Area Number 21K18195
Research Category

Grant-in-Aid for Challenging Research (Pioneering)

Allocation TypeMulti-year Fund
Review Section Medium-sized Section 29:Applied condensed matter physics and related fields
Research InstitutionTokyo Institute of Technology

Principal Investigator

Sannomiya Takumi  東京工業大学, 物質理工学院, 准教授 (60610152)

Co-Investigator(Kenkyū-buntansha) 石井 あゆみ  早稲田大学, 理工学術院, 准教授 (70406833)
秋葉 圭一郎  国立研究開発法人量子科学技術研究開発機構, 高崎量子応用研究所 量子機能創製研究センター, 主幹研究員 (80712538)
Project Period (FY) 2021-07-09 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥25,870,000 (Direct Cost: ¥19,900,000、Indirect Cost: ¥5,970,000)
Fiscal Year 2023: ¥5,200,000 (Direct Cost: ¥4,000,000、Indirect Cost: ¥1,200,000)
Fiscal Year 2022: ¥10,530,000 (Direct Cost: ¥8,100,000、Indirect Cost: ¥2,430,000)
Fiscal Year 2021: ¥10,140,000 (Direct Cost: ¥7,800,000、Indirect Cost: ¥2,340,000)
Keywordsカソードルミネセンス / 相関計測 / 透過電子顕微鏡 / 時間相関 / 電子顕微鏡
Outline of Research at the Start

蛍光寿命顕微鏡においては、光の回折限界に起因して、分子・原子レベルでの機能が重要となる100nm以下の情報が得られない。最近の超解像法等によって分解能の向上は試みられているものの、数十nmが限界である。本研究では、光子ー光子相関および電子ー光子相関測定という全く新しい計測手法により、蛍光寿命顕微鏡による回折限界を打破する。この手法では、電子プローブの空間分解能で測定可能であり、既存の光による寿命顕微鏡の分解能をはるかにしのぐ。高い空間分解能を生かした透過電子顕微鏡ベースの計測によりナノ構造の同時計測・直接対比も可能となる。

Outline of Final Research Achievements

Due to the diffraction limit of light, fluorescence lifetime microscopy cannot not provide insights into features below 100 nm scales, which are crucial when investigating the functions at molecular or atomic levels. In this research, we established a microscopy technique that surpasses this limit by introducing a novel approach in electron microscopy: photon-photon correlation and electron-photon correlation measurements utilizing electron beam-excited luminescence (cathodoluminescence). This innovative method eliminates the need for pulsing the electron beam and enables the measurement of luminescence lifetime with the spatial resolution inherent to the electron probe. By conducting photon-photon correlation mapping and electron-photon correlation mapping, we successfully visualized the distribution of luminescent centers and defects in semiconductors, shedding light on their lifetime dynamics.

Academic Significance and Societal Importance of the Research Achievements

本申請で開発する寿命イメージングは、自然放出される電子1つをパルスとして利用し、パルス電子銃を必要としないパッシブな計測で、発光寿命を検出系を組み込むだけで簡便に実現ができるため、広い汎用性を持つ。パルス電子銃を用いた従来の方法と異なり、電子光学系がそのままであるので、電子顕微鏡本来の分解能(光の2桁上)で発光イメージングができ、同時計測された試料内部の構造と直接比較可能である。さらに、本研究の手法では、発光のプロセスや相関の強度を表す重要なパラメタも同時に得られるため、学術的にも新奇な知見が得られている。

Report

(5 results)
  • 2023 Annual Research Report   Final Research Report ( PDF )
  • 2022 Research-status Report
  • 2021 Comments on the Screening Results   Research-status Report
  • Research Products

    (40 results)

All 2024 2023 2022 2021

All Journal Article (5 results) (of which Int'l Joint Research: 1 results,  Peer Reviewed: 5 results,  Open Access: 3 results) Presentation (34 results) (of which Int'l Joint Research: 11 results,  Invited: 7 results) Patent(Industrial Property Rights) (1 results) (of which Overseas: 1 results)

  • [Journal Article] Cathodoluminescence spectral and lifetime mapping of Cs<sub>4</sub>PbBr<sub>6</sub>: fast lifetime and its scintillator application2024

    • Author(s)
      Kubota Tetsuya、Yanagimoto Sotatsu、Saito Hikaru、Akiba Keiichirou、Ishii Ayumi、Sannomiya Takumi
    • Journal Title

      Applied Physics Express

      Volume: 17 Issue: 1 Pages: 015005-015005

    • DOI

      10.35848/1882-0786/ad1bc4

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Diffusion-Dominated Luminescence Dynamics of CsPbBr3 Studied Using Cathodoluminescence and Microphotoluminescence Spectroscopy2024

    • Author(s)
      Sho Nekita, Sotatsu Yanagimoto, Takumi Sannomiya, Keiichirou Akiba, Masato Takiguchi, Hisashi Sumikura, Itsuki Takagi, Kazutaka G. Nakamura, SenPo Yip, You Meng, Johnny C. Ho, Tetsuya Okuyama, Mitsuhiro Murayama, Hikaru Saito
    • Journal Title

      Nano Letters

      Volume: 24 Issue: 13 Pages: 3971-3977

    • DOI

      10.1021/acs.nanolett.4c00483

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Time-correlated electron and photon counting microscopy2023

    • Author(s)
      Yanagimoto Sotatsu、Yamamoto Naoki、Yuge Tatsuro、Saito Hikaru、Akiba Keiichirou、Sannomiya Takumi
    • Journal Title

      Communications Physics

      Volume: 6 Issue: 1 Pages: 260-260

    • DOI

      10.1038/s42005-023-01371-1

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Focused light introduction into transmission electron microscope via parabolic mirror2023

    • Author(s)
      Adachi Yoshikazu、Yamamoto Naoki、Sannomiya Takumi
    • Journal Title

      Ultramicroscopy

      Volume: 251 Pages: 113759-113759

    • DOI

      10.1016/j.ultramic.2023.113759

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Superbunching in cathodoluminescence: A master equation approach2023

    • Author(s)
      Yuge Tatsuro、Yamamoto Naoki、Sannomiya Takumi、Akiba Keiichirou
    • Journal Title

      Physical Review B

      Volume: 107 Issue: 16 Pages: 165303-165303

    • DOI

      10.1103/physrevb.107.165303

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Presentation] プラズモニクスにおけるカソードルミネセンスの光子相関計測の活用2024

    • Author(s)
      柳本宗達, 山本直紀、三宮工、秋葉圭一郎
    • Organizer
      第4回次世代プラズモニック化学への挑戦
    • Related Report
      2023 Annual Research Report
  • [Presentation] 低温カソードルミネセンス法によるCs4PbBr6の観察2024

    • Author(s)
      久保田哲矢、柳本宗達、斉藤光、秋葉圭一郎、石井あゆみ、三宮工
    • Organizer
      第71回応用物理学会春季学術講演会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Accessing Light by Electron Beam: Cathodoluminescence2023

    • Author(s)
      T. Sannomiya
    • Organizer
      日本顕微鏡学会第79回学術講演会
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] 誘電体球を用いた透過電子顕微鏡内での電子線照射による温度上昇の計測2023

    • Author(s)
      安達 良和、Izzah Machfuudzoh、杉本 泰、藤井 稔、三宮 工
    • Organizer
      日本顕微鏡学会第79回学術講演会
    • Related Report
      2023 Annual Research Report
  • [Presentation] 異なるCs4PbBr6試料のカソードルミネセンスマッピング2023

    • Author(s)
      久保田哲矢、柳本宗達、斉藤光、秋葉圭一郎、石井あゆみ、三宮工
    • Organizer
      日本顕微鏡学会第79回学術講演会
    • Related Report
      2023 Annual Research Report
  • [Presentation] 高速電子と放出光子の時間相関計測2023

    • Author(s)
      柳本 宗達、山本 直紀、弓削 達郎、斉藤 光、秋葉 圭一郎、三宮 工
    • Organizer
      日本顕微鏡学会第79回学術講演会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Carrier diffusion effect in temporal decay of cathodoluminescence: toward nanoscale characterization of carrier dynamics2023

    • Author(s)
      Sho Nekita, Sotatsu Yanagimoto, Tetsuya Kubota, Takumi Sannomiya, Keiichirou Akiba, Masato Takiguchi, Hisashi Sumikura, Itsuki Takagi, Kazutaka G.Nakamura, Senpo Yip, You Meng, Johnny C. Ho, Tetsuya Okuyama, Mitsuhiro Murayama,?Hikaru Saito
    • Organizer
      The 20th International Microscopy Congress
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Cathodoluminescence Spectrum and Lifetime Mapping of Cs4PbBr62023

    • Author(s)
      Tetsuya Kubota, Sotatsu Yanagimoto, Hikaru Saito, Keiichirou Akiba, Ayumi Ishii, Takumi Sannomiya
    • Organizer
      The 20th International Microscopy Congress
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Monitoring temperature increase by laser and electron beam irradiation using a dielectric sphere in TEM2023

    • Author(s)
      Yoshikazu Adachi, Izzah Machfuudzoh, Hiroshi Sugimoto, Minoru Fujii, Takumi Sannomiya
    • Organizer
      The 20th International Microscopy Congress
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Demonstration of the Time-Correlated Electron and Photon Counting Microscopy2023

    • Author(s)
      Sotatsu Yanagimoto, Naoki Yamamoto, Tatsuro Yuge, Hikaru Saito, Keiichirou Akiba, Takumi Sannomiya
    • Organizer
      The 20th International Microscopy Congress
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 電子線をパルス化しない時間分解カソードルミネセンス計測2023

    • Author(s)
      三宮工
    • Organizer
      日本顕微鏡学会第66回シンポジウム
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] Analysis of Trench Defects in InGaN Single Quantum Well by Photon Correlation Mapping2023

    • Author(s)
      Sotatsu Yanagimoto, Naoki Yamamoto, Takumi Sannomiya, Keiichirou Akiba
    • Organizer
      2023 Tokyo Institute of Technology - Dalian University of Technology Joint Workshop on Advanced Materials and Chemical Technology
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Monitoring temperature increase by laser and electron beam irradiation using Si sphere in TEM2023

    • Author(s)
      Yoshikazu Adachi, Izzah Machfuudzoh, Hiroshi Sugimoto, Minoru Fujii, Takumi Sannomiya
    • Organizer
      2023 Tokyo Institute of Technology - Dalian University of Technology Joint Workshop on Advanced Materials and Chemical Technology
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 電子線を用いたナノスケール光計測2023

    • Author(s)
      三宮工
    • Organizer
      ナノプローブテクノロジー第167委員会105回研究会
    • Related Report
      2022 Research-status Report
    • Invited
  • [Presentation] 侵入酸素によるCsPbBr3のバンドギャップの拡大2023

    • Author(s)
      根北 翔、辻 雄太、柳本 宗達、三宮 工、秋葉 圭一郎、Yip Sen Po、Meng You、Ho Johnny、村山光宏、斉藤 光
    • Organizer
      第70回応用物理学会春季学術講演会
    • Related Report
      2022 Research-status Report
  • [Presentation] カソードルミネセンスを用いたCs4PbBr6のナノスケール発光寿命計測2023

    • Author(s)
      久保田哲矢、柳本宗達、斉藤光、秋葉圭一郎、石井あゆみ、三宮工
    • Organizer
      第70回応用物理学会春季学術講演会
    • Related Report
      2022 Research-status Report
  • [Presentation] 高速電子線検出器応答にむけたCsPbBr3のサブナノ秒CL2022

    • Author(s)
      根北 翔,柳本 宗達,三宮 工,秋葉 圭一郎,滝口 雅人,角倉 久史,村山 光宏,斉藤 光
    • Organizer
      日本顕微鏡学会第78回学術講演会
    • Related Report
      2022 Research-status Report
  • [Presentation] カソードルミネセンス光子相関マッピングによる InGaN量子井戸の発光寿命解析2022

    • Author(s)
      柳本 宗達,山本 直紀,三宮 工,秋葉 圭一郎
    • Organizer
      日本顕微鏡学会第78回学術講演会
    • Related Report
      2022 Research-status Report
  • [Presentation] Cs4PbBr6のカソードルミネセンスにおける発光寿命測定とシンチレータ応用2022

    • Author(s)
      久保田 哲矢,柳本 宗達,斉藤 光,秋葉 圭一郎,石井 あゆみ,三宮 工
    • Organizer
      日本顕微鏡学会第78回学術講演会
    • Related Report
      2022 Research-status Report
  • [Presentation] Analysis of the Purcell effect of nitrogen-vacancy centers in nanodiamonds coupled to Ag nanostructures2022

    • Author(s)
      S. Yanagimoto, N. Yamamoto, T. Sannomiya, K. Akiba
    • Organizer
      The 13th Asia-Pacific Conference on Near-Field Optics
    • Related Report
      2022 Research-status Report
    • Int'l Joint Research
  • [Presentation] Chiral light emission from circular plasmonic hole controlled by electron beam2022

    • Author(s)
      T. Sannomiya, T. Matsukata
    • Organizer
      The 13th Asia-Pacific Conference on Near-Field Optics
    • Related Report
      2022 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] 光子相関マッピングを用いたInGaN量子井戸のトレンチ欠陥における発光劣化機構の解析2022

    • Author(s)
      柳本 宗達,山本 直紀,三宮 工,秋葉 圭一郎
    • Organizer
      第83回応用物理学会秋季学術講演会
    • Related Report
      2022 Research-status Report
  • [Presentation] 走査型透過電子顕微鏡カソードルミネセンスによる光子相関計測2022

    • Author(s)
      柳本 宗達,山本 直紀,三宮 工,秋葉 圭一郎
    • Organizer
      創発の場-フォトニクス討論会
    • Related Report
      2022 Research-status Report
  • [Presentation] Photon correlation measurement at the nanoscale by STEM cathodoluminescence2022

    • Author(s)
      柳本 宗達,山本 直紀,三宮 工,秋葉 圭一郎
    • Organizer
      日本顕微鏡学会 若手研究部会
    • Related Report
      2022 Research-status Report
  • [Presentation] 透過電子顕微鏡カソードルミネセンスによるナノスケール光解析2022

    • Author(s)
      三宮 工
    • Organizer
      表面真空学会九州支部セミナー
    • Related Report
      2022 Research-status Report
    • Invited
  • [Presentation] CsPbBr3ナノワイヤの蛍光のサイズ依存性の起源2022

    • Author(s)
      根北 翔 , 柳本 宗達 , 三宮 工 , 秋葉 圭一郎, 滝 口 雅人 , 角倉 久史 , Meng You , Yip Sen Po , Ho Johnny C, 斉藤 光
    • Organizer
      第69回応用物理学会春季学術講演会
    • Related Report
      2021 Research-status Report
  • [Presentation] 電子線によるCsPbBr3のサブナノ秒発光2022

    • Author(s)
      根北 翔 , 柳本 宗達 , 三宮 工 , 秋葉 圭一郎, 滝 口 雅人, 角倉 久史 , 斉藤 光
    • Organizer
      第69回応用物理学会春季学術講演会
    • Related Report
      2021 Research-status Report
  • [Presentation] Cathodoluminescence with Interference2021

    • Author(s)
      T. Sannomiya
    • Organizer
      EBSN
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] タイコグラフィーによる位相回復への中間レンズの焦点はずれの影響と補正2021

    • Author(s)
      三石 和貴,三宮 工
    • Organizer
      日本顕微鏡学会
    • Related Report
      2021 Research-status Report
  • [Presentation] STEMカソードルミネセンスにおける光子相関計測2021

    • Author(s)
      柳本 宗達,山本 直紀,三宮 工,秋葉 圭一郎
    • Organizer
      日本顕微鏡学会
    • Related Report
      2021 Research-status Report
  • [Presentation] ナノダイヤモンド中の窒素‐空孔中心の銀ナノ構造との結合に伴うパーセル効果の解析2021

    • Author(s)
      柳本 宗達,山本 直紀,三宮 工,秋葉 圭一郎
    • Organizer
      第82回応用物理学会秋季学術講演会
    • Related Report
      2021 Research-status Report
  • [Presentation] 電子顕微顕微鏡へ導入した光の点像分布関数2021

    • Author(s)
      安達 良和、三宮 工
    • Organizer
      第82回応用物理学会秋季学術講演会
    • Related Report
      2021 Research-status Report
  • [Presentation] Visualization of Optical Field by Electron Microscopy2021

    • Author(s)
      T. Sannomiya
    • Organizer
      2021 Sino-Japan Young Scholar Forum on Advanced Materials and Related Techonologies
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Analysis of the Purcell Effect of Nitrogen-Vacancy Centers in Nanodiamonds Coupled to Ag Nanostructures2021

    • Author(s)
      S. Yanagimoto, N. Yamaomoto, T. Sannomiya, K. Akiba
    • Organizer
      2021 Sino-Japan Young Scholar Forum on Advanced Materials and Related Techonologies
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research
  • [Patent(Industrial Property Rights)] 電子顕微鏡、電子ー光子創刊測定装置、及び電子ー光子相関測定方法2022

    • Inventor(s)
      三宮工、柳本宗達、秋葉圭一郎、斉藤光
    • Industrial Property Rights Holder
      三宮工、柳本宗達、秋葉圭一郎、斉藤光
    • Industrial Property Rights Type
      特許
    • Filing Date
      2022
    • Related Report
      2021 Research-status Report
    • Overseas

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Published: 2021-07-13   Modified: 2025-01-30  

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