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2019 Fiscal Year Annual Research Report

液体の超高速光電子分光による溶液化学反応の研究

Research Project

Project/Area Number 15H05753
Research InstitutionKyoto University

Principal Investigator

鈴木 俊法  京都大学, 理学研究科, 教授 (10192618)

Co-Investigator(Kenkyū-buntansha) 足立 俊輔  京都大学, 理学研究科, 准教授 (90431874)
山本 遥一  京都大学, 理学研究科, 助教 (70837319)
Project Period (FY) 2015-05-29 – 2020-03-31
Keywords光電子分光 / 超高速分光 / 溶液化学 / 極端紫外光 / 高次高調波発生 / 溶媒和電子 / 光化学 / 放射線化学
Outline of Annual Research Achievements

液体の紫外超高速光電子分光では、溶液中で発生した電子が非弾性散乱されて運動エネルギーを一部失う効果が問題となり、我々の2019年のScience Advancesの論文でこれを解決するSpectral Retrieval法を開発したところである。
極端紫外光を用いれば非弾性散乱が無視できるほど低減できるため、本年度はこれを実践し、I-から水、メタノール、エタノールへの電荷移動反応を極端紫外光電子分光で観測し、非弾性散乱の無視できる状態で観測した結果とSpetral Retrievalが一致することを確認した。
シクロヘキサジエン(CHD)の開環反応は、ノーベル化学賞の対象となったWoodward-Hoffmann則に従う反応であり、太陽光の下でのビタミンDの生合成に関係する。この反応は分子の二電子励起状態を経た非断熱遷移によるものと理論的に予測されていたが、実験的には同定されていなかった。我々は世界で初めてフィラメンテーション四光波混合で発生した極端紫外光と高次高調波発生による極短極端紫外光を組み合わせ、48fsという極めて短い交差相関時間を実現し、紫外光パルスで1、3-シクロヘキサジエンを光励起し、1、3、5-ヘキサトリエンへの開環反応を極端紫外光電子分光で追跡した。光励起によって生成される一電子励起状態が約30fs後に二電子励起状態に変化し、70fs以内にC-C結合が開裂してヘキサトリエンが生成する様子が極めて明瞭に観測された。また、生成したヘキサトリエンは振動量子ビートを明瞭に示した。
実験結果解析のためCardiff大学のKnowles教授らが行ったXMS-CASPT2レベルのポテンシャルエネルギー曲面上の古典軌跡計算にXMS-CASPT2レベルの光イオン化動力学計算を組み合わせて実験結果を再現できた。
2020年7月末瞬時電力低下によるレーザー破損のため3月まで延長した。

Research Progress Status

令和元年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

令和元年度が最終年度であるため、記入しない。

  • Research Products

    (27 results)

All 2021 2020 2019 Other

All Journal Article (15 results) (of which Int'l Joint Research: 5 results,  Peer Reviewed: 15 results,  Open Access: 1 results) Presentation (11 results) (of which Int'l Joint Research: 8 results,  Invited: 4 results) Remarks (1 results)

  • [Journal Article] Design and characterization of a magnetic bottle electron spectrometer for time-resolved extreme UV and X-ray photoelectron spectroscopy of liquid microjets2021

    • Author(s)
      N. Kurahashi, S. Thuermer, S. Y. Liu, Y. Yamamoto, S. Karashima, A. Bhattacharya, Y. Ogi, T. Horio, and T. Suzuki
    • Journal Title

      Structural Dynamics

      Volume: - Pages: -

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Ultafast extreme ultraviolet photoelectron spectroscopy of nonadiabatic photodissociation of CS2 from 1B2(1Σu+) state: product formation via an intermediate electronic state2021

    • Author(s)
      S. Karashima, Y-I Suzuki, and T. Suzuki
    • Journal Title

      Journal of Physical Chemistry Letters

      Volume: 12 Pages: 3755-3761

    • DOI

      10.1021/acs.jpclett.1c00864

    • Peer Reviewed
  • [Journal Article] Spiers Memorial Lecture: Introduction to ultrafast spectroscopy and imaging of photochemical reactions2021

    • Author(s)
      Toshinori Suzuki
    • Journal Title

      Faraday Discussions

      Volume: - Pages: -

    • DOI

      10.1039/D1FD00015B

    • Peer Reviewed
  • [Journal Article] Valence Photoelectron Spectra of Liquid Methanol and Ethanol Measured Using He II Radiation2021

    • Author(s)
      S. Thuermer, S. Takatoshi, and S. Toshinori
    • Journal Title

      The Journal of Physical Chemistry A

      Volume: 125 Pages: 2492-2503

    • DOI

      10.1021/acs.jpca.1c00288

    • Peer Reviewed
  • [Journal Article] Femtosecond X-ray emission study if the spin cross-over dynamics in haem proteins2020

    • Author(s)
      D. Linschel et al, and T. Suzuki
    • Journal Title

      Nature Communication

      Volume: 11 Pages: 4145

    • DOI

      10.1038/s41467-020-17923-w.

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Ultrafast Dynamics of Water Radiolysis: Hydrated Electron Formation, Solvation, Recombination, and Scavenging2020

    • Author(s)
      Y. Yamamoto, T. Suzuki
    • Journal Title

      The Journal of Physical Chemistry Letters

      Volume: 11 Pages: 5510-5516

    • DOI

      10.1021/acs.jpclett.0c01468

    • Peer Reviewed
  • [Journal Article] Surface potential of liquid microjet investigated using extreme ultraviolet photoelectron spectroscopy2020

    • Author(s)
      J. Nishitani, S. Karashima, C. W. West, and T. Suzuki
    • Journal Title

      Journal of Chemical Physics

      Volume: 152 Pages: 144503

    • DOI

      10.1063/5/0005930

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Extreme ultraviolet time-resolved photoelectron spectroscopy of aqueous aniline solution: enhanced surface concentration and pump-induced space charge effect2020

    • Author(s)
      C. W. West, J. Nishitani, C. Higashimura, and T. Suzuki
    • Journal Title

      Molecular Physics

      Volume: - Pages: e1748240

    • DOI

      10.1080/00268976.2020.1748240

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Methyl substitution effects on the non-adiabatic dynamics of benzene: lifting three-state quasi-degeneracy at conical intersections2020

    • Author(s)
      S. Adachi and T. Suzuki
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 22 Pages: 2814-2818

    • DOI

      10.1039/c9cp06164a

    • Peer Reviewed
  • [Journal Article] Time-resolved photoelectron imaging of acetone with 9.3 eV photoexcitation2019

    • Author(s)
      R. Uenishi, T. Horio, and T. Suzuki
    • Journal Title

      Journal of Physical Chemistry A

      Volume: 123 Pages: 6848-6853

    • DOI

      10.1021/acs.jpca.9b05179

    • Peer Reviewed
  • [Journal Article] Solvated electron formation from the conduction band of liquid methanol: transformation from a shallow to deep trap state2019

    • Author(s)
      A. Hara, Y. Yamamoto, and T. Suzuki
    • Journal Title

      Journal of Chemical Physics

      Volume: 151 Pages: 114503

    • DOI

      10.1063/1.5116818

    • Peer Reviewed
  • [Journal Article] Ultrafast internal conversion and solvation of electrons in water, methanol and ethanol2019

    • Author(s)
      S. Karashima, Y. Yamamoto, and T. Suzuki
    • Journal Title

      Journal of Physical Chemistry Letters

      Volume: 10 Pages: 4499-4504

    • DOI

      10.1021/acs.jpclett.9b01750

    • Peer Reviewed
  • [Journal Article] Charge-transfer-to-solvent reaction in a hydrophobic tetrabutylammonium iodide molecular layer in aqueous solution2019

    • Author(s)
      S. Karashima and T. Suzuki
    • Journal Title

      Journal of Physical Chemistry B

      Volume: 123 Pages: 3769-3775

    • DOI

      10.1021/acs.jpcb.8b12210

    • Peer Reviewed
  • [Journal Article] Binding energy of solvated electrons and retrieval of true UV photoelectron spectra of liquids2019

    • Author(s)
      J. Nishitani, Y. Yamamoto, C. W. West, S. Karashima, and T. Suzuki
    • Journal Title

      Science Advances

      Volume: 5 Pages: eaaw6896

    • DOI

      10.1126/sciadv.aaw6896

    • Peer Reviewed / Open Access
  • [Journal Article] Probing ultrafast dynamics during and after passing through conical intersections2019

    • Author(s)
      S. Adachi, T. Schatteburg, A. Humeniuk, R. Mitric, and T. Suzuki
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 21 Pages: 13902-13905

    • DOI

      10.1039/c8cp04426k

    • Peer Reviewed / Int'l Joint Research
  • [Presentation] Observation of electronic and structural dynamics in photochemical reactions2020

    • Author(s)
      T.Suzuki
    • Organizer
      Time-resolved imaging of photo-induced dynamics Faraday Discussion of Royal Society of Chemistry
    • Int'l Joint Research / Invited
  • [Presentation] 液体の超高速光電子分光とスペクトル回復法による溶媒和電子の束縛エネルギーと非断熱遷移の研究2020

    • Author(s)
      山本遥一
    • Organizer
      日本化学会第100回春季年会
    • Int'l Joint Research
  • [Presentation] Ultrafast VUV photoelectron spectroscopy of non-adiabatic dynamics in the gas and condensed phases2019

    • Author(s)
      T.Suzuki
    • Organizer
      The 26th Colloquium on High-Resolution Molecular Spectroscopy (HRMS Dijon 2019)
    • Int'l Joint Research / Invited
  • [Presentation] 液体の超高速光電子分光におけるスペクトル回復法の開発と溶媒和電子への適用2019

    • Author(s)
      鈴木 俊法
    • Organizer
      第13回分子科学討論会
  • [Presentation] Ultrafast photoelectron spectroscopy of solvated electrons2019

    • Author(s)
      T.Suzuki
    • Organizer
      The 35th International Symposium on Free Radicals
    • Int'l Joint Research / Invited
  • [Presentation] 水の窓軟X線を用いた液相での過渡吸収分光実現に向けた装置開発2019

    • Author(s)
      足立俊輔
    • Organizer
      第80回応用物理学会秋季学術講演会
  • [Presentation] 溶媒和電子の束縛エネルギーの決定とスペクトル回復法の開発2019

    • Author(s)
      山本遥一
    • Organizer
      原子衝突学会第44会年会
  • [Presentation] Binding energies of solvated electrons and retrieval of true photoelectron spectra of liquids2019

    • Author(s)
      T.Suzuki
    • Organizer
      XXVIIIth International Symposium on Molecular Beams (ISMB2019)
    • Int'l Joint Research / Invited
  • [Presentation] Solvated Electron Formation from Conduction Band of Liquid Methanol2019

    • Author(s)
      T.Suzuki
    • Organizer
      第35回化学反応討論会
    • Int'l Joint Research
  • [Presentation] Time-Resolved Photoelectron Spectroscopy of Acetone with 9.3 eV Photoexcitation2019

    • Author(s)
      T. Horio
    • Organizer
      第35回化学反応討論会
    • Int'l Joint Research
  • [Presentation] Non-adiabatic dynamics of benzene and its methy1 derivatives studied by vacuum-UV time-resolved photoelectron spectroscopy2019

    • Author(s)
      足立俊輔
    • Organizer
      第35回化学反応討論会
    • Int'l Joint Research
  • [Remarks] 京都大学大学院 理学研究科 化学専攻 物理化学研究室hp

    • URL

      http://kuchem.kyoto-u.ac.jp/bukka/

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Published: 2021-12-27  

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