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Elucidation of photoionization process in condensed phase by using multiple excitation and development to high-efficiency electron transfer process

Research Project

Project/Area Number 21H01889
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 32010:Fundamental physical chemistry-related
Research InstitutionOsaka University

Principal Investigator

Miyasaka Hiroshi  大阪大学, エマージングサイエンスデザインR3センター, 特任教授 (40182000)

Co-Investigator(Kenkyū-buntansha) 五月女 光  大阪大学, 大学院基礎工学研究科, 助教 (60758697)
Project Period (FY) 2021-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥17,810,000 (Direct Cost: ¥13,700,000、Indirect Cost: ¥4,110,000)
Fiscal Year 2023: ¥2,210,000 (Direct Cost: ¥1,700,000、Indirect Cost: ¥510,000)
Fiscal Year 2022: ¥4,290,000 (Direct Cost: ¥3,300,000、Indirect Cost: ¥990,000)
Fiscal Year 2021: ¥11,310,000 (Direct Cost: ¥8,700,000、Indirect Cost: ¥2,610,000)
Keywords電子移動 / 光イオン化 / 多重励起過程 / フェムト秒ダイナミクス / ピコ秒ダイナミクス / 多光子吸収 / 光誘起電子移動 / 多重励起 / 逐次二光子吸収
Outline of Research at the Start

光誘起電子移動は光エネルギー変換や光物質変換にも深く関わる過程であり、その高効率化は重要な課題である。このためには、励起状態寿命の間に迅速に反応が進行し電荷分離状態が高収率で生成すること、後続反応のためには電荷分離状態が高エネルギーを持ち、かつ再結合反応が遅いことの3条件が必要となる。しかし電子移動反応速度は始終状態間のエネルギー差に依存し、3条件を同時に満足することは一般的には困難であった。本研究では、多重励起により生成した高位励起状態を利用し長距離の電子供与体-受容体間の電荷分離反応を進行させることで、2光子を利用した上記3条件を満たす新規高効率電荷分離状態生成手法の開拓と確立をめざす。

Outline of Final Research Achievements

In the photoionization process in the condensed phase, the initial distance between the parent cation and the ejected electron has been estimated to be several nanometers. In the case that the electrons in such ionized states or their precursors can be quickly and efficiently captured by other molecules and, as a result, the long distance is fixed, it is expected that a high-energy level charge-separated state with a long interionic distance can be rapidly generated and, consequently, the charge recombination can be suppressed. In this research, we utilized highly electronic excited states generated by pulsed laser multiple excitation methods in various solution systems and realized the formation of charge-separated states with long interionic distances by the ultrafast (< 1 ps) electron capture. In addition, we have revealed the mechanism of the unique electronic state that enables low-energy ionization, and factors that determine the cation-electron distance.

Academic Significance and Societal Importance of the Research Achievements

本研究では、天然光合成系のZスキームと原理は異なるが、逐次2光子吸収によるイオン化を進行させ、放出電子を迅速かつ効率良く他分子に捕捉させ距離を固定化することで、後続の還元・酸化等の反応を誘起できる高エネルギーかつ再結合を抑制した電荷分離状態を高収率で実現した。これは、光エネルギー変換や人工光合成にも深く関わる光誘起電子移動反応におけるエネルギーギャップ則の制限により、従来は困難であった(1) 迅速な電荷分離反応、(2) 高エネルギーな電荷分離状態、(3) 遅い再結合を同時に満足できる新手法であり、光誘起電子移動反応の利用に対して重要な方法を示した。

Report

(4 results)
  • 2023 Annual Research Report   Final Research Report ( PDF )
  • 2022 Annual Research Report
  • 2021 Annual Research Report
  • Research Products

    (25 results)

All 2024 2023 2022 2021 Other

All Int'l Joint Research (1 results) Journal Article (9 results) (of which Int'l Joint Research: 3 results,  Peer Reviewed: 8 results,  Open Access: 1 results) Presentation (14 results) (of which Int'l Joint Research: 8 results,  Invited: 8 results) Book (1 results)

  • [Int'l Joint Research] Lille University/Paris-Saclay高等師範学校(フランス)

    • Related Report
      2021 Annual Research Report
  • [Journal Article] Nanoscopic Photomechanical Motion of Small Particles Induced by Optical Force due to Positive and Negative Photo-absorption by Excited States of Molecules2024

    • Author(s)
      Syoji Ito, Takato Mizoguchi, Masato Mori, Masafumi Koga, Hikaru Sotome, Mamoru Tamura, Hajime Ishihara, Hiroshi Miyasaka
    • Journal Title

      J. Phys. Chem. C

      Volume: 128 Issue: 12 Pages: 5206-5214

    • DOI

      10.1021/acs.jpcc.3c08495

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Reaction Dynamics of Molecules in Highly Electronically Excited States Attained by Multiphoton and Multiple Excitation Methods2023

    • Author(s)
      Hiroshi Miyasaka, Syoji Ito, Hikaru Sotome
    • Journal Title

      Pure Appl. Chem.

      Volume: 95 Issue: 8 Pages: 921-929

    • DOI

      10.1515/pac-2023-0205

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Fluctuation-mediated orbital rotation of microparticles in non-coaxially counter-propagating optical tweezers2023

    • Author(s)
      Kenji Setoura, Takayasu kakimoto, Hiroshi Miyasaka, Syoji Ito
    • Journal Title

      Photochem. Photobiol. Sci.

      Volume: 22 Issue: 11 Pages: 2519-2526

    • DOI

      10.1007/s43630-023-00465-7

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Dynamics and mechanism of radical formation in a highly sensitive oxime photoinitiator as revealed by time-resolved absorption and EPR measurements2023

    • Author(s)
      Sameshima Kaori、Kawakami Tomomi、Sotome Hikaru、Fuki Masaaki、Kobori Yasuhiro、Miyasaka Hiroshi
    • Journal Title

      Journal of Photochemistry and Photobiology A: Chemistry

      Volume: 437 Pages: 114479-114479

    • DOI

      10.1016/j.jphotochem.2022.114479

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Femtosecond Dynamics of Stepwise Two-Photon Ionization in Solutions as Revealed by Pump-Repump-Probe Detection with Burst Mode of Photoexcitation2022

    • Author(s)
      Hikaru Sotome, Masafumi Koga, Tomoya Sawada, Hiroshi Miyasaka
    • Journal Title

      Phys. Chem. Chem. Phys.

      Volume: - Issue: 23 Pages: 14187-14197

    • DOI

      10.1039/d1cp03866d

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Direct Detection of Long-Range Interdomain Auger Recombination in Dumbbell-Shaped Quasi-Type-II Nanoparticle2022

    • Author(s)
      Masafumi Koga, Ko Masuoka, Shuhei Tsuneizumi, Tatsuya Kameyama, Syoji Ito, Tsukasa Torimoto, and Hiroshi Miyasaka
    • Journal Title

      J Phys. Chem. Lett.

      Volume: 13 Issue: 29 Pages: 6845-6851

    • DOI

      10.1021/acs.jpclett.2c01077

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 多重励起技術による光誘起電荷分離状態の計測と形成2022

    • Author(s)
      五月女 光, 宮坂 博
    • Journal Title

      光化学

      Volume: 53 Pages: 155-158

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Direct Determination of Molar Absorption Coefficients of Several Molecules in the Lowest Excited Singlet States2021

    • Author(s)
      Masafumi Koga, Hikaru Sotome, Naoki Ide, Syoji Ito, Yutaka Nagasawa, Hiroshi Miyasaka
    • Journal Title

      Photochem. Photobiol. Sci.

      Volume: 20 Issue: 10 Pages: 1287-1297

    • DOI

      10.1007/s43630-021-00104-z

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 凝縮系における高い電子励起状態からの反応過程2021

    • Author(s)
      宮坂 博, 五月女 光
    • Journal Title

      光化学

      Volume: 52 Pages: 46-53

    • NAID

      40022683678

    • Related Report
      2021 Annual Research Report
  • [Presentation] hotochemical Processes in Higher Excited States Produced by Multiphoton Absorption and Multiple Excitation2023

    • Author(s)
      Hiroshi Miyasaka
    • Organizer
      10th International Symposium on Photochromism
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] iffusion Dynamics of Electron Ejected by Photoionization in Solution: Relation with the Fluctuation of the Solvent2023

    • Author(s)
      Yuya Hirata, Tomoya Sawada, Hikaru Sotome, Hiroshi Miyasaka
    • Organizer
      The 31st International Conference on Photochemistry
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 高い電子易動度をもつ溶媒中の光イオン化と放出電子の拡散・再結合ダイナミクス2023

    • Author(s)
      平田 裕矢, 澤田 知弥, 五月女 光, 宮坂 博
    • Organizer
      2023年光化学討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] 液相多光子イオン化における放出電子の拡散ダイナミクス:電子易動度との相関2023

    • Author(s)
      澤田 知弥, 五月女 光, 宮坂 博
    • Organizer
      日本化学会 第103春季年会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 多光子イオン化により生成したカチオン-電子対の再結合ダイナミクス:電子易動度と対間距離分布の相関2022

    • Author(s)
      澤田 知弥, 五月女 光, 宮坂 博
    • Organizer
      第16回分子科学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Photochemical Processes in Higher Excited States Attained via Multiphoton Absorption and Multiple Excitation in the Condensed Phase2022

    • Author(s)
      Hiroshi Miyasaka
    • Organizer
      International Congress on Pure & Applied Chemistry
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Photochemical Processes in Higher Excited States Produced by Multiphoton Absorption and Multiple Excitation in the Condensed Phase2022

    • Author(s)
      Hiroshi Miyasaka
    • Organizer
      VII Iberian Photochemistry Conference
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Ultrafast Multiphoton Spectroscopy of Higher Excited States2022

    • Author(s)
      Hiroshi Miyasaka
    • Organizer
      28th IUPAC Symposium on Photochemistry
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 超短パルスレーザーによる凝縮相分子系の多重光子応答過程の研究2022

    • Author(s)
      宮坂 博
    • Organizer
      日本化学会 第102春季年会
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] Ultrafast Dynamics of Multiphoton Ionization and Electron Capture in Solutions2021

    • Author(s)
      Hiroshi Miyasaka
    • Organizer
      The International Chemical Congress of Pacific Basin Societies 2021
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Advanced Ultrafast Multiphoton Laser Spectroscopy on Photochemical Molecular Processes in Higher Excited States in the Condensed Phase2021

    • Author(s)
      Hiroshi Miyasaka
    • Organizer
      Asian Photochemistry Conference
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Ultrafast Dynamics of Multiphoton Ionization and Electron Capture in Solutions2021

    • Author(s)
      Hiroshi Miyasaka
    • Organizer
      6th Nanosynergetics Workshop
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 液相芳香族化合物の光イオン化により生成したカチオン-電子対の超高速ダイナミクス2021

    • Author(s)
      ○澤田 知弥, 古賀 雅史, 五月女 光, 神戸 正雄, 菅 晃一, 吉田 陽一, 伊都 将司, 宮坂 博
    • Organizer
      第15回分子科学討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 多重励起を利用したCdTe 量子ドットの光イオン化ダイナミクスの解明2021

    • Author(s)
      ○井出 直樹, 古賀 雅史, 三宅 友斗, 五月女 光, 宮坂 博
    • Organizer
      2021年光化学討論会
    • Related Report
      2021 Annual Research Report
  • [Book] パルスレーザーによる化学反応の時間分解計測2023

    • Author(s)
      宮坂 博、五月女 光、石橋千英
    • Total Pages
      133
    • Publisher
      共立出版
    • Related Report
      2023 Annual Research Report

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Published: 2021-04-28   Modified: 2025-01-30  

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