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Investigating the shape of reactive potential energy surfaces using ultrafast coherent vibrational spectroscopy

Research Project

Project/Area Number 21H01895
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 InstitutionInstitute for Molecular Science

Principal Investigator

Kuramochi Hikaru  分子科学研究所, 協奏分子システム研究センター, 准教授 (40709367)

Project Period (FY) 2021-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥17,420,000 (Direct Cost: ¥13,400,000、Indirect Cost: ¥4,020,000)
Fiscal Year 2023: ¥2,860,000 (Direct Cost: ¥2,200,000、Indirect Cost: ¥660,000)
Fiscal Year 2022: ¥6,890,000 (Direct Cost: ¥5,300,000、Indirect Cost: ¥1,590,000)
Fiscal Year 2021: ¥7,670,000 (Direct Cost: ¥5,900,000、Indirect Cost: ¥1,770,000)
Keywords超高速分光 / 電子励起状態 / 多次元分光 / コヒーレンス / 非線形分光 / ラマン分光
Outline of Research at the Start

化学反応は多くの自由度から成る複雑なポテンシャルエネルギー曲面上で起こるため,その形状を知り,反応座標を明らかにすることは化学反応研究における究極の目標の一つである.しかし,凝縮相多原子分子の反応性ポテンシャルエネルギー曲面に関する情報を実験的に得る事は極めて困難であった.本研究では,極短パルスを用いたコヒーレント分子振動の時間領域観測に基づく先端的な超高速分光法を開発・駆使することで,反応座標や振動モード間の非調和カップリング,円錐交差を形成する振動モードなど,反応性ポテンシャルエネルギー曲面の形状を決定づける情報を実験的に得ることを目指す.

Outline of Final Research Achievements

We developed a new light source to generate <10 fs pulses in the ultraviolet to near-infrared region. Based on this light source, two-dimensional Raman spectroscopy for observing the couplings between excited-state vibrational modes and a pump-probe spectroscopy with extreme time resolution have been developed. In 2D Raman spectroscopy of TIPS-pentacene, a typical system that shows singlet exciton fission, the obtained data suggested the existence of couplings between the excited-state vibrational modes, which cannot be explained by a simple harmonic oscillator model. The present project succeeded in establishing a technological basis for obtaining new knowledge on electronic excited states that cannot be obtained by conventional methods.

Academic Significance and Societal Importance of the Research Achievements

電子励起状態における振動モード間のカップリングは,反応が起こるポテンシャルエネルギー曲面の形状を決定づける重要なパラメータであるが,従来の実験手法ではこうした情報を得ることは極めて困難であった.本研究で開発を進めた新しい分光手法によってこうした情報が実験的に得られるようになったことは,大きな学術的意義がある.先端的な分光計測法の開発により,化学反応ダイナミクス研究の新しい可能性を開拓した.

Report

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

    (28 results)

All 2023 2022 2021

All Journal Article (8 results) (of which Int'l Joint Research: 3 results,  Peer Reviewed: 8 results) Presentation (20 results) (of which Int'l Joint Research: 3 results,  Invited: 4 results)

  • [Journal Article] Photoexcited Plasmon-Driven Ultrafast Dynamics of the Adsorbate Probed by Femtosecond Time-Resolved Surface-Enhanced Time-Domain Raman Spectroscopy2023

    • Author(s)
      Kumar Pardeep、Kuramochi Hikaru、Takeuchi Satoshi、Tahara Tahei
    • Journal Title

      The Journal of Physical Chemistry Letters

      Volume: 14 Issue: 11 Pages: 2845-2853

    • DOI

      10.1021/acs.jpclett.2c03813

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Spectroscopic mapping of the gold complex oligomers (dimer, trimer, tetramer, and pentamer) by excited-state coherent nuclear wavepacket motion in aqueous solutions2023

    • Author(s)
      M. Iwamura, R. Urayama, A. Fukui, K. Nozaki, L. Liu, H. Kuramochi, S. Takeuchi, T. Tahara
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 25 Issue: 2 Pages: 966-974

    • DOI

      10.1039/d2cp04823j

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] フェムト秒時間分解時間領域ラマン分光で観る光化学反応の超高速構造ダイナミクス2022

    • Author(s)
      倉持 光、田原 太平
    • Journal Title

      光化学

      Volume: 53 Pages: 132-137

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] フェムト秒時間分解インパルシブ誘導ラマン分光による光誘起結合生成ダイナミクスの実時間構造追跡2022

    • Author(s)
      倉持光、竹内佐年、岩村宗高、田原太平
    • Journal Title

      光学

      Volume: 51 Pages: 8-14

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Excited-state proton transfer dynamics in LSSmOrange studied by time-resolved impulsive stimulated Raman spectroscopy2021

    • Author(s)
      P. Kumar, E. Fron, H. Hosoi, H. Kuramochi, S. Takeuchi, H. Mizuno, T. Tahara
    • Journal Title

      Journal of Physical Chemistry Letters

      Volume: 12 Issue: 31 Pages: 7466-7473

    • DOI

      10.1021/acs.jpclett.1c01653

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Tracking Ultrafast Structural Dynamics by Time-Domain Raman Spectroscopy2021

    • Author(s)
      Kuramochi Hikaru、Tahara Tahei
    • Journal Title

      Journal of the American Chemical Society

      Volume: 143 Issue: 26 Pages: 9699-9717

    • DOI

      10.1021/jacs.1c02545

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Skeletal structure of the chromophore of photoactive yellow protein in the excited state investigated by ultraviolet femtosecond stimulated Raman spectroscopy2021

    • Author(s)
      H. Kuramochi, S. Takeuchi, H. Kamikubo, M. Kataoka, T. Tahara
    • Journal Title

      Journal of Physical Chemistry B

      Volume: 125 Issue: 23 Pages: 6154-6161

    • DOI

      10.1021/acs.jpcb.1c02828

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Femtosecond Structural Dynamics of Complex Molecular Systems Studied by Time-Domain Raman Spectroscopy Using Few-Cycle Pulses2021

    • Author(s)
      Kuramochi Hikaru
    • Journal Title

      Molecular Science

      Volume: 15 Issue: 1 Pages: A0117

    • DOI

      10.3175/molsci.15.A0117

    • NAID

      130008079181

    • ISSN
      1881-8404
    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Presentation] コロイドZnSナノ結晶に配位したペリレンビスイミド誘導体の疑可逆的な光脱離2023

    • Author(s)
      吉岡 大祐,米田 勇祐,I-Ya Chang,倉持 光,金 賢得,小林 洋一
    • Organizer
      日本化学会 第103春季年会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 発光性ジラジカルが形成するエキシマー的励起種の電子状態解明2023

    • Author(s)
      松岡 亮太,米田 勇祐,倉持 光,三浦 智明,生駒 忠昭,西郷 将生,江原 巧,宮田 潔志,恩田 健,草本 哲郎
    • Organizer
      日本化学会 第103春季年会
    • Related Report
      2022 Annual Research Report
  • [Presentation] チエニルジケトン誘導体の光励起に伴う配座ダイナミクスと高速項間交差2023

    • Author(s)
      木村 周慈,江原 巧,宮田 潔志,米田 勇祐,倉持 光,谷 洋介,恩田 健
    • Organizer
      日本化学会 第103春季年会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Al(III)二核三重螺旋錯体のJahn-Teller歪みを伴う発光機構の解明2023

    • Author(s)
      江原 巧,宮田 潔志,小野 利和,村中 厚哉,米田 勇祐,倉持 光,恩田 健
    • Organizer
      日本化学会 第103春季年会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 半導体ナノ結晶の表面有機配位子の擬可逆的光脱離過程2022

    • Author(s)
      小林 洋一, 吉岡 大祐, 米田勇祐, 倉持 光, 金 賢得
    • Organizer
      ナノ学会第20回大会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Quasi-reversible photoelimination of organic ligands on semiconductor nanocrystals2022

    • Author(s)
      Daisuke Yoshioka, Yusuke Yoneda, Yoshinori Okayasu, Yuki Nagai, Hikaru Kuramochi, Hyeom-Deuk Kim, Yoichi Kobayashi
    • Organizer
      2022年光化学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] フェムト秒過渡吸収で観測されるジシアノ金会合体の核波束運動と水溶液の濃度依存性2022

    • Author(s)
      岩村 宗高,野崎 浩一,Li Liu,倉持 光,竹内 佐年,田原 太平
    • Organizer
      第16回分子科学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] サブ10フェムト秒パルスを用いた過渡2次元電子分光法による水和電子の不均一性の観測2022

    • Author(s)
      松崎 維信,倉持 光,田原 太平
    • Organizer
      第16回分子科学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Ultrafast structural changes of large [Au(CN)2]- oligomers in triplet excited state observed by femtosecond time-resolved impulsive stimulated Raman spectroscopy2022

    • Author(s)
      Li Liu, Hikaru Kuramochi, Munetaka Iwamura, Koichi Nozaki, Tahei Tahara
    • Organizer
      第16回分子科学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] ZnSナノ結晶の表面有機配位子の擬可逆的光脱離過程の解明2022

    • Author(s)
      吉岡 大祐,米田 勇祐,倉持 光,金 賢得,小林 洋一
    • Organizer
      第16回分子科学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 水溶液中におけるジシアノ金(I)錯体の励起5量体から5量体の時間分解吸収・発光および振動スペクトル2022

    • Author(s)
      岩村宗高,浦山里奈,福井愛理,野﨑浩一, Li Liu,倉持 光,竹内佐年,田原太平
    • Organizer
      第33回配位化合物の光化学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Ultrafast Excited-state Dynamics in Au Hexa-core Clusters Observed by Femtosecond Time-resolved Absorption Spectroscopy2022

    • Author(s)
      Tsukasa Takanashi, Honoka Watanabe, Munetaka Iwamura, Koichi Nozaki, Yukatsu Shichibu, Katsuaki Konishi, Hikaru Kuramochi, Tahei Tahara
    • Organizer
      the 24th International Symposium on the Photochemistry and Photophysics of Coordination Compounds (ISPPCC)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Ultrafast Dynamics of Platinum(II) Complex Oligomers2022

    • Author(s)
      Munetaka Iwamura, Honoka Watanabe, Koichi Nozaki, Tsukasa Takanashi, Hikaru Kuramochi, Tahei Tahara
    • Organizer
      the 24th International Symposium on the Photochemistry and Photophysics of Coordination Compounds (ISPPCC)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Mapping multi-dimensional excited-state dynamics using nonlinear electronic and vibrational spectroscopy2022

    • Author(s)
      Hikaru Kuramochi
    • Organizer
      ACS Publications Summit: The Journal of Physical Chemistry Letters
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Mapping Structural Dynamics in Photochemistry with Ultrafast Nonlinear Spectroscopy2022

    • Author(s)
      Hikaru Kuramochi
    • Organizer
      日本化学会 第102春季年会 Asian International Symposium - Photochemistry -
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] 数サイクルパルスを用いた極限分光計測による複雑分子系のフェムト秒構造化学研究2021

    • Author(s)
      倉持光
    • Organizer
      第15回 分子科学討論会
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] フェムト秒時間分解吸収分光による金六核クラスターにおける超高速励起状態ダイナミクスの観測2021

    • Author(s)
      高梨司、渡邊ほのか、岩村宗高、野崎浩一、七分勇勝、小西克明、倉持光、田原太平
    • Organizer
      第15回 分子科学討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Vibration of large K[Au(CN)2] oligomers (tetramer and pentamer) in the excited triplet state observed by time-resolved impulsive stimulated Raman spectroscopy2021

    • Author(s)
      Li Liu, Hikaru Kuramochi, Munetaka Iwamura, Koichi Nozaki, Tahei Tahara
    • Organizer
      第15回 分子科学討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Real-time control of liquid crystalline adhesive by turning ultraviolet light on and off2021

    • Author(s)
      Tomoaki Konishi, Yuri Saida, Wataru Yajima, Ryo Shikata, Masaki Hada, Yuushi Shimoda, Kiyoshi Miyata, Yusuke Yoneda, Hikaru Kuramochi, Yumi Nakaike, Mitsuo Hara, Ryuma Sato, Takuya Yamakado, Ryota Kotani, Shohei Saito
    • Organizer
      2021年 光化学討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 数サイクルパルスで観る機能性複雑分子の超高速電子・構造ダイナミクス2021

    • Author(s)
      倉持光
    • Organizer
      M&BE研究会「時代を切り拓く有機分子・バイオエレクトロニクス」
    • Related Report
      2021 Annual Research Report
    • Invited

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

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