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Direct observation for steric effect in chemical reaction by controlling molecular orientation of reactants

Research Project

Project/Area Number 17KT0008
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeMulti-year Fund
Section特設分野
Research Field Transition State Control
Research InstitutionOsaka University

Principal Investigator

CHE DOCK-CHIL  大阪大学, 理学研究科, 講師 (20273732)

Project Period (FY) 2017-07-18 – 2021-03-31
Project Status Completed (Fiscal Year 2020)
Budget Amount *help
¥18,330,000 (Direct Cost: ¥14,100,000、Indirect Cost: ¥4,230,000)
Fiscal Year 2019: ¥2,600,000 (Direct Cost: ¥2,000,000、Indirect Cost: ¥600,000)
Fiscal Year 2018: ¥7,410,000 (Direct Cost: ¥5,700,000、Indirect Cost: ¥1,710,000)
Fiscal Year 2017: ¥8,320,000 (Direct Cost: ¥6,400,000、Indirect Cost: ¥1,920,000)
Keywords配向状態選別 / 光解離 / 反応分岐比 / ベクトル相関 / ハロタン / イソハロエタン / 反応遷移状態 / 分子の配向制御 / 生成物の散乱分布 / 生成物の速度分布 / 生成物の反応分岐 / 六極不均一電場 / ハロタン分子 / 二次元画像計測システム / 分子の配向状態選別 / 配向制御 / 遷移状態の直接観測
Outline of Final Research Achievements

Photodissociation dynamics of halothane molecule state-selected using a hexapolar was studied at 235 nm laser light. The scattering distribution of competitively formed Br and Cl atoms was determined by a two-dimensional imaging technique. As a result, it was found that the Br atom is formed by the direct dissociation, and the Cl atom has two formation pathways. It was found that the reaction branching ratio of Cl atom formation is about twice as large as that of Br atom. This is different from the results predicted from the conventional dissociation energy and absorption spectrum correlated atoms, and suggests that a new dissociation mechanism needs to be considered. On the other hand, the direction of the transition dipole moment in the photoexcitation of isohaloethane was experimentally determined by selecting the orientation state and examining the correlation with the polarization vector of the laser.

Academic Significance and Societal Importance of the Research Achievements

ハロタン分子の光解離の研究を実施し、競争的に生成するBr及びCl原子生成の反応機構を解明した。反応分岐比を測定したところ、Cl原子生成はBr原子に比べ反応分岐比が大きいことが明らかとなった。この結果は、結合エネルギーや分子の吸収スペクトルから予測される結果と全く異なり、新しい解離メカニズムの必要性を提案する結果であった。一方で、対象軸を持たない分子の遷移モーメントの方向を調べることは困難とされていた。今回、イソハロタン分子の双極子モーメントとレーザーの偏光ベクトルのベクトル相関を調べることで分子が光を吸収する際の遷移双極子モーメントの方向を実験的に決定することに成功した。

Report

(5 results)
  • 2020 Annual Research Report   Final Research Report ( PDF )
  • 2019 Research-status Report
  • 2018 Research-status Report
  • 2017 Research-status Report
  • Research Products

    (22 results)

All 2020 2019 2018 2017 Other

All Int'l Joint Research (8 results) Journal Article (8 results) (of which Int'l Joint Research: 5 results,  Peer Reviewed: 8 results,  Open Access: 5 results) Presentation (5 results) (of which Int'l Joint Research: 3 results) Book (1 results)

  • [Int'l Joint Research] ペルージャ大学(イタリア)

    • Related Report
      2020 Annual Research Report
  • [Int'l Joint Research] 台湾大学/原子分子科学研究所(その他の国・地域(台湾))

    • Related Report
      2020 Annual Research Report
  • [Int'l Joint Research] ペルージャ大学(イタリア)

    • Related Report
      2019 Research-status Report
  • [Int'l Joint Research] 台湾大学/原子分子科学研究所(その他の国・地域)

    • Related Report
      2019 Research-status Report
  • [Int'l Joint Research] ペルージャ大学(イタリア)

    • Related Report
      2018 Research-status Report
  • [Int'l Joint Research] 台湾大学/原子分子科学研究所(台湾)

    • Related Report
      2018 Research-status Report
  • [Int'l Joint Research] 台湾大学/原子分子科学研究所(台湾)

    • Related Report
      2017 Research-status Report
  • [Int'l Joint Research] ペルージャ大学(イタリア)

    • Related Report
      2017 Research-status Report
  • [Journal Article] UV Photodissociation of Halothane in a Focused Molecular Beam: Space-Speed Slice Imaging of Competitive Bond Breaking into Spin-Orbit-Selected Chlorine and Bromine Atoms2020

    • Author(s)
      Che Dock-Chil、Nakamura Masaaki、Chang Hsiu-Pu、Lin King-Chuen、Kasai Toshio、Aquilanti Vincenzo、Palazzetti Federico
    • Journal Title

      The Journal of Physical Chemistry A

      Volume: 124 Issue: 26 Pages: 5288-5296

    • DOI

      10.1021/acs.jpca.0c02800

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Stereodynamic Imaging of Bromine Atomic Photofragments Eliminated from 1-Bromo-2-methylbutane Oriented via Hexapole State Selector2019

    • Author(s)
      Nakamura Masaaki、Chang Hsiu-Pu、Lin King-Chuen、Kasai Toshio、Che Dock-Chil、Palazzetti Federico、Aquilanti Vincenzo
    • Journal Title

      The Journal of Physical Chemistry A

      Volume: 123 Issue: 31 Pages: 6635-6644

    • DOI

      10.1021/acs.jpca.9b04048

    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Vectorial imaging of the photodissociation of 2-bromobutane oriented via hexapolar state selection2019

    • Author(s)
      Nakamura Masaaki、Palazzetti Federico、Tsai Po-Yu、Yang Shiun-Jr、Lin King-Chuen、Kasai Toshio、Che Dock-Chil、Lombardi Andrea、Aquilanti Vincenzo
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 21 Issue: 26 Pages: 14164-14172

    • DOI

      10.1039/c8cp04270e

    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Roaming and chaotic behaviors in collisional and photo-initiated beam reactions: A role of nearby network dynamics in quantum/classical world2018

    • Author(s)
      Toshio Kasai, Dock-Chil Che, Po-Yu Tsai, Masaaki Nakamura, Balaganesh Muthiah, King-Chuen Lin
    • Journal Title

      Rendiconti Lincei. Scienze Fisiche e Naturali

      Volume: 29 Issue: 2 Pages: 219-232

    • DOI

      10.1007/s12210-018-0709-4

    • Related Report
      2018 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Atomic force microscopy analysis of SasA-KaiC complex formation involved in information transfer from the KaiABC clock machinery to the output pathway in cyanobacteria2018

    • Author(s)
      Murakami Reiko、Hokonohara Hitomi、Che Dock-Chil、Kawai Tomoji、Matsumoto Takuya、Ishiura Masahiro
    • Journal Title

      Genes to Cells

      Volume: 23 Issue: 4 Pages: 294-306

    • DOI

      10.1111/gtc.12574

    • Related Report
      2018 Research-status Report 2017 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Roaming and chaotic behaviors in collisional and photo-initiated beam reactions: A role of nearby network dynamics in quantum/classical world2018

    • Author(s)
      Toshio KASAI, Dock-Chil Che, Po-Yu Tsai, Masaaki Nakamura, Balaganesh Muthiah and King-Chuen Lin
    • Journal Title

      Rendiconti Lincei

      Volume: -

    • Related Report
      2017 Research-status Report
    • Peer Reviewed
  • [Journal Article] Stereodirectional images of molecules oriented by a variable-voltage hexapolar field: Fragmentation channels of 2-bromobutane electronically excited at two photolysis wavelengths2017

    • Author(s)
      Nakamura Masaaki、Yang Shiun-Jr、Lin King-Chuen、Kasai Toshio、Che Dock-Chil、Lombardi Andrea、Palazzetti Federico、Aquilanti Vincenzo
    • Journal Title

      The Journal of Chemical Physics

      Volume: 147 Issue: 1 Pages: 013917-013917

    • DOI

      10.1063/1.4981025

    • Related Report
      2017 Research-status Report
    • Peer Reviewed
  • [Journal Article] Rotational state-selection and alignment of chiral molecules by electrostatic hexapoles2017

    • Author(s)
      Palazzetti Federico、Lombardi Andrea、Nakamura Masaaki、Yang Shiun-Jr.、Kasai Toshio、Lin King-Chuen、Tsai Po-Yu、Che Dock-Chil
    • Journal Title

      AIP Conference Proceedings

      Volume: 1790 Pages: 020019-020019

    • DOI

      10.1063/1.4968645

    • Related Report
      2017 Research-status Report
    • Peer Reviewed
  • [Presentation] Photodissociation dynamics of oriented halot hane2019

    • Author(s)
      Che, D.-C., Nakamura, M, K.-C. Lin, T. Kasai, K.-C. Lin, F. Palazzetti, V. Aquilanti
    • Organizer
      反応討論会2019
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] ハロタンの光解離によるBr及びCl原子生成の反応分岐機構の解明2019

    • Author(s)
      蔡 徳七,中村 雅明、 笠井 俊夫,K.-C. Lin, F. Palazzetti, V. Aquilanti
    • Organizer
      応用物理学会2019
    • Related Report
      2019 Research-status Report
  • [Presentation] 配向状態を選別したハロタン分子の光解離ダイナミクス2018

    • Author(s)
      蔡 徳七,中村 雅明,笠井 俊夫,Lin King-Chuen
    • Organizer
      第12回分子科学討論会2018福岡
    • Related Report
      2018 Research-status Report
  • [Presentation] Photodissociation dynamics of oriented halothane using hexapole electric field2018

    • Author(s)
      CHE Dock-Chil, NAKAMURA Masaaki, KASAI Toshio, LIN King-Chuen
    • Organizer
      第34回化学反応討論会
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] Photodissociation dynamics of spatially-oriented asymmetric top molecules2018

    • Author(s)
      NAKAMURA Masaaki, CHANG Hsiu-Pu,LIN King-Chuen, KASAI Toshio, CHE Dock-Chil, LOMBARDI Andrea, PALAZZETTI Federico,AQUILANTI Vincenz
    • Organizer
      第34回化学反応討論会
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Book] Space and speed Slice Imaging of Molecular Photdissociation: Stereodirectionality and Chirality2020

    • Author(s)
      F. Palazzetti, A. Lombardi, M. Nakamura, P.-Y. Tsai, D.-C. Che, T. Kasai, K.-C. Lin, V. Aquilanti
    • Publisher
      Accademia Nazionale delle Scienze detta dei XL
    • ISBN
      9788898075386
    • Related Report
      2020 Annual Research Report

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Published: 2017-07-21   Modified: 2022-12-28  

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