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Development of a spectroscopy beyond the time-energy restriction and microscopic approach to solvation dynamics.

Research Project

Project/Area Number 16H06028
Research Category

Grant-in-Aid for Young Scientists (A)

Allocation TypeSingle-year Grants
Research Field Physical chemistry
Research InstitutionTokyo Institute of Technology

Principal Investigator

Miyazaki Mitsuhiko  東京工業大学, 科学技術創成研究院, 助教 (00378598)

Project Period (FY) 2016-04-01 – 2019-03-31
Project Status Completed (Fiscal Year 2018)
Budget Amount *help
¥19,500,000 (Direct Cost: ¥15,000,000、Indirect Cost: ¥4,500,000)
Fiscal Year 2018: ¥3,250,000 (Direct Cost: ¥2,500,000、Indirect Cost: ¥750,000)
Fiscal Year 2017: ¥7,280,000 (Direct Cost: ¥5,600,000、Indirect Cost: ¥1,680,000)
Fiscal Year 2016: ¥8,970,000 (Direct Cost: ¥6,900,000、Indirect Cost: ¥2,070,000)
Keywords時間分解赤外分光 / 溶媒和クラスター / 溶媒和ダイナミクス / 分子分光
Outline of Final Research Achievements

In this work, a new time-resolved infrared spectroscopy that enables us to achieve picosecond time resolution and nanosecond energy resolution, utilizing pico- and nano- second lasers. This method was applied to solvated clusters in the gas phase to investigate solvation dynamics from individual molecular point of view.
It was clarified that mechanism of solvation dynamics is classified into two-cases; repulsive and attractive cases depending on the solute-solvent interaction potential. In both cases, intracluster vibrational energy redistribution (IVR) plays a key role. It is important, however, that the direction of the energy flow is opposite. It was also found that the solvation dynamics rate can change more than three-orders of magnitude for the two cases.

Academic Significance and Societal Importance of the Research Achievements

化学反応では、反応物だけでなくそれを取り囲む溶媒分子の運動が反応機構、速度に大きな影響を与える。しかし、溶媒分子は大量に存在するため、一つ一つの溶媒分子の運動に基づいて溶媒運動の役割を研究することはできていない。
本研究で開発した時間・エネルギー極限分光法の開発と溶媒和クラスターへの適用は、一つ一つの溶媒分子の運動を区別して測定する手段を提供できる。この手法により得られる結果は、化学反応機構の分子論的理解の基礎を与えるほか、理論計算のベンチマークとしても重要な意味を持つ。生体反応で重要であると予想されている特異的に強い相互作用を持つ溶媒分子の役割を理解するための基礎としても重要である。

Report

(4 results)
  • 2018 Annual Research Report   Final Research Report ( PDF )
  • 2017 Annual Research Report
  • 2016 Annual Research Report
  • Research Products

    (29 results)

All 2019 2018 2017 2016 Other

All Int'l Joint Research (4 results) Journal Article (12 results) (of which Int'l Joint Research: 8 results,  Peer Reviewed: 12 results,  Acknowledgement Compliant: 2 results) Presentation (12 results) (of which Int'l Joint Research: 6 results,  Invited: 4 results) Remarks (1 results)

  • [Int'l Joint Research] Technische Universitaet Berlin(ドイツ)

    • Related Report
      2018 Annual Research Report
  • [Int'l Joint Research] ベルリン工科大学/ウルツブルグ大学(ドイツ)

    • Related Report
      2017 Annual Research Report
  • [Int'l Joint Research] エクスマルセイユ大学(フランス)

    • Related Report
      2017 Annual Research Report
  • [Int'l Joint Research] ベルリン工科大学(ドイツ)

    • Related Report
      2016 Annual Research Report
  • [Journal Article] Effect of alkali ions on optical properties of flavins: Vibronic spectra of cryogenic M+lumiflavin complexes (M = Li-Cs)2019

    • Author(s)
      David Mueller, Pablo Nieto, Mitsuhiko Miyazaki, and Otto Dopfer
    • Journal Title

      Faraday Discussions

      Volume: 印刷中 Pages: 256-275

    • DOI

      10.1039/c8fd00203g

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Electron-proton transfer mechanism of excited-state hydrogen transfer in phenol-(NH3)n (n=5) studied by delayed ionization detected femtosecond time-resolved NIR spectroscopy2018

    • Author(s)
      Mitsuhiko Miyazaki, Nozomi Washio, and Masaaki Fujii
    • Journal Title

      Chemical Physics

      Volume: 515 Pages: 580-585

    • DOI

      10.1016/j.chemphys.2018.08.004

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Effect of alkali ions on optical properties of flavins: vibronic spectra of cryogenic M+lumichrome ions (M = Li-Cs) in the gas phase2018

    • Author(s)
      Pablo Nieto, David Mueller, Alexander Sheldrick, Alan Guenther, Mitsuhiko Miyazaki, and Otto Dopfer
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 20 Issue: 34 Pages: 22148-22158

    • DOI

      10.1039/c8cp03950j

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] A theoretical study on the size-dependence of ground-state proton transfer in phenol-ammonia clusters2018

    • Author(s)
      Shimizu Toshihiko、Hashimoto Kenro、Hada Masahiko、Miyazaki Mitsuhiko、Fujii Masaaki
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 20 Issue: 5 Pages: 3265-3276

    • DOI

      10.1039/c7cp05247b

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Stepwise Microhydration of Aromatic Amide Cations: Solvation Networks Revealed by Infrared Spectra of Acetanilide+-(H2O)n Clusters (n<=3)2018

    • Author(s)
      J. Klyne, M. Schmies, M. Miyazaki, M. Fujii, O. Dopfer
    • Journal Title

      Phys. Chem. Chem. Phys.

      Volume: 20 Issue: 5 Pages: 3148-3164

    • DOI

      10.1039/c7cp04659f

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Sequential Microhydration of Cationic 5-Hydroxyindole (5HI+): Infrared Photodissociation Spectra of 5HI+-Wn Clusters (W=H2O, n<=4)2018

    • Author(s)
      J. Klyne, M. Miyazaki, M. Fujii, O. Dopfer
    • Journal Title

      Phys. Chem. Chem. Phys.

      Volume: 20 Issue: 5 Pages: 3092-3108

    • DOI

      10.1039/c7cp06132c

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Real-time observation of the photoionization-induced water rearrangement dynamics in the 5-hydroxyindole-water cluster by time-resolved IR spectroscopy2018

    • Author(s)
      Mitsuhiko Miyazaki, Ayumi Naito, Takamasa Ikeda, Johanna Klyne, Kenji Sakota, Hiroshi Sekiya, Otto Dopfer, Masaaki Fujii
    • Journal Title

      Phys. Chem. Chem. Phys.

      Volume: 20 Issue: 5 Pages: 3079-3091

    • DOI

      10.1039/c7cp06127g

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Electron-Proton Transfer Mechanism of Excited-State Hydrogen Transfer in Phenol-(NH3)n (n=3 and 5)2017

    • Author(s)
      Miyazaki Mitsuhiko、Ohara Ryuhei、Dedonder Claude、Jouvet Christophe、Fujii Masaaki
    • Journal Title

      Chemistry - A European Journal

      Volume: 24 Issue: 4 Pages: 881-890

    • DOI

      10.1002/chem.201704129

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] A structural study on the excimer state of an isolated benzene dimer using infrared spectroscopy in the skeletal vibration region2017

    • Author(s)
      Miyazaki Mitsuhiko、Fujii Masaaki
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 19 Issue: 34 Pages: 22759-22776

    • DOI

      10.1039/c7cp03480f

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Deciphering environment effects in peptide bond solvation dynamics by experiment and theory2017

    • Author(s)
      Wohlgemuth Matthias、Miyazaki Mitsuhiko、Tsukada Kohei、Weiler Martin、Dopfer Otto、Fujii Masaaki、Mitric Roland
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 19 Issue: 33 Pages: 22564-22572

    • DOI

      10.1039/c7cp03992a

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Theoretical Study on the Size-Dependence of Ground-State Proton Transfer in 1-Naphthol-Ammonia Clusters2016

    • Author(s)
      T. Shimizu, M. Miyazaki, M. Fujii
    • Journal Title

      J. Chem. Phys. A

      Volume: 120 Issue: 36 Pages: 7167-7174

    • DOI

      10.1021/acs.jpca.6b07079

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Photoionization-induced π-H site switching dynamics in phenol+-Rg (Rg = Ar, Kr) dimers probed by picosecond time-resolved infrared spectroscopy2016

    • Author(s)
      M. Miyazaki, Y. Sakata, M. Schutz, O. Dopfer, M. Fujii
    • Journal Title

      Phys. Chem. Chem. Phys.

      Volume: 18 Issue: 35 Pages: 24746-24754

    • DOI

      10.1039/c6cp05016f

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Int'l Joint Research / Acknowledgement Compliant
  • [Presentation] Water migration dynamics in hydrated clusters -- Real-time observation by time-resolved IR spectroscopy --2019

    • Author(s)
      Mitsuhiko Miyazaki
    • Organizer
      日本化学会第99春季年会
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] IR dip分光法による4-メチルホルムアニリド‐水1:1クラスターにおけるイオン化誘起水分子マイグレーションの観測2018

    • Author(s)
      紙谷 大陸、今野 裕貴、大塚 玲美奈、宮﨑 充彦、藤井 正明
    • Organizer
      第12回分子科学討論会
    • Related Report
      2018 Annual Research Report
  • [Presentation] Real-time observation of slow water rearrangement dynamics in the 5-hydroxyindole-water cluster cation by time-resolved IR spectroscopy2018

    • Author(s)
      Mitsuhiko Miyazaki, Ayumi Naito, Takamasa Ikeda, Hiroshi Sekiya, Johanna Klyne, Otto Dopfer, Masaaki Fujii
    • Organizer
      Gordon Research Conferences: Molecular and Ionic Clusters 2018
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] IR dip分光法による4-メチルホルムアニリド・水1:1クラスターにおけるイオン化誘起水分子マイグレーション反応の観測2018

    • Author(s)
      紙谷 大陸、宮崎 充彦、石川 春樹、藤井 正明
    • Organizer
      日本化学会第98春季年会
    • Related Report
      2017 Annual Research Report
  • [Presentation] Real-time observation of charge transfer dynamics in a (p-cyanophenyl)pentamethyldisilane-water cluster by picosecond time-resolved IR spectroscopy2017

    • Author(s)
      Mitsuhiko Miyazaki, Saori Matsuyama, Haruki Ishikawa, and Masaaki Fujii
    • Organizer
      XVIII Time Resolved Vibrational Spectroscopy 2017
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Photo-induced charge transfer and hydration dynamics in a (p-cyanophenyl)pentamethyldisilane-water cluster by picosecond time-resolved IR spectroscopy2017

    • Author(s)
      Mitsuhiko Miyazaki, Saori Matsuyama, Haruki Ishikawa, and M. Fujii
    • Organizer
      International Symposium on Molecular Beams 2017
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Photoexcitation induced water reorientation dynamics in the 5-hydroxyindole-water cluster studied by time resolved IR spectroscopy2017

    • Author(s)
      M. Miyazaki, A. Naito, J. Klyne, O. Dopfer, and M. Fujii
    • Organizer
      Bunsentagung 2017 116th General Assembly of the German Bunsen Society for Physical Chemistry
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] ピコ秒時間分解赤外分光法による(p-シアノフェニル)ペンタメチルジシラン-水1:2クラスターの溶媒再配向過程の実時間観測2017

    • Author(s)
      今野 祐貴、石川 春樹、宮﨑 充彦、藤井 正明
    • Organizer
      第11回分子科学討論会
    • Related Report
      2017 Annual Research Report
  • [Presentation] フーリエ限界を回避した気相ピコ秒時間分解赤外分光法の開発-アセトアニリド-水クラスターにおけるイオン化誘起水移動反応への適用-2017

    • Author(s)
      小野 純平、宮﨑 充彦、小野 愛真、紙谷 大陸、石川 春樹、藤井 正明
    • Organizer
      第11回分子科学討論会
    • Related Report
      2017 Annual Research Report
  • [Presentation] Photoionization-induced water reorientation in the 5-hydroxyindole water cluster -A challenge to real-time observation of slow dynamics-2016

    • Author(s)
      Mitsuhiko Miyazaki
    • Organizer
      The 20th East Asian Workshop on Chemical Dynamics
    • Place of Presentation
      National Sun Yat Sen University, Kaohsiung, Taiwan
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] ピコ秒時間分解分光による分子クラスターを用いた化学反応素過程への構造論的アプローチ2016

    • Author(s)
      宮﨑 充彦
    • Organizer
      第十回分子科学討論会
    • Place of Presentation
      神戸ファッションマート、兵庫県神戸市
    • Related Report
      2016 Annual Research Report
    • Invited
  • [Presentation] 5-ヒドロキシインドール水和クラスターの時間分解赤外分光 ―イオン化誘起異性化反応ダイナミクスの実時間観測―2016

    • Author(s)
      内藤 あゆみ、宮崎 充彦、迫田 憲治、関谷 博、藤井 正明
    • Organizer
      第十回分子科学討論会
    • Place of Presentation
      神戸ファッションマート、兵庫県神戸市
    • Related Report
      2016 Annual Research Report
  • [Remarks] 最新の研究

    • URL

      http://www.res.titech.ac.jp/news/reserch/

    • Related Report
      2018 Annual Research Report

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Published: 2016-04-21   Modified: 2020-03-30  

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