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A spectroscopic study on hemibonds in gas phase clusters

Research Project

Project/Area Number 18H01931
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 InstitutionTohoku University

Principal Investigator

Fujii Asuka  東北大学, 理学研究科, 教授 (50218963)

Project Period (FY) 2018-04-01 – 2021-03-31
Project Status Completed (Fiscal Year 2020)
Budget Amount *help
¥17,550,000 (Direct Cost: ¥13,500,000、Indirect Cost: ¥4,050,000)
Fiscal Year 2020: ¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2019: ¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2018: ¥9,230,000 (Direct Cost: ¥7,100,000、Indirect Cost: ¥2,130,000)
Keywords半結合 / ラジカル / カチオン / クラスター / 赤外分光 / 分子分光 / 非調和振動 / フェルミ共鳴 / 2中心3電子結合 / 硫化水素 / 2中心3電子結合 / ラジカルカチオン / プロトン移動 / 水素結合
Outline of Final Research Achievements

The hemibond is a nonclassical covalent bond, in which three electrons are shared by two centers (atoms). Roles of the hemibond in radiation chemistry and biochemistry have attracted much interest. In the present study, microsolvation effects on the hemibond between hydrogen sulfide were investigated by infrared spectroscopy of model clusters in the gas phase. It was shown that the hemibond is stable to microsolvation by a single water molecules, but solvation by a single alcohol molecule easily breaks the hemibond. In addition, a new type of hemibond was found between hydrogen sulfide and pi electrons of benzene. This hemibond is a good benchmark to test the validity of density functionals to simulate hemibonds.

Academic Significance and Societal Importance of the Research Achievements

これまで専ら凝集相におけるブロードな可視・紫外吸収という多様な解釈が可能な実験データーに基づいて議論されていた半結合研究に構造を直接反映する赤外分光手法と理論計算と比較可能な気相モデルクラスター手法を適用し、精度の高い半結合研究を可能とした。これにより、これまでの半結合研究にあった曖昧さを排し、厳密かつ確度の高い議論が出来るようになった。半結合はアルツハイマー病発症の機構にも関与しているとされており、将来的には本研究の知見を出発点として医学的な応用も期待される。

Report

(4 results)
  • 2020 Annual Research Report   Final Research Report ( PDF )
  • 2019 Annual Research Report
  • 2018 Annual Research Report
  • Research Products

    (41 results)

All 2021 2020 2019 2018 Other

All Int'l Joint Research (4 results) Journal Article (18 results) (of which Int'l Joint Research: 11 results,  Peer Reviewed: 18 results) Presentation (18 results) (of which Int'l Joint Research: 6 results,  Invited: 5 results) Remarks (1 results)

  • [Int'l Joint Research] 原子輿分子科學研究所(その他の国・地域  台湾)

    • Related Report
      2020 Annual Research Report
  • [Int'l Joint Research] Tata Institute of Fundamental Research(インド)

    • Related Report
      2019 Annual Research Report
  • [Int'l Joint Research] National Chiao Tung University(その他の国・地域)

    • Related Report
      2019 Annual Research Report
  • [Int'l Joint Research] Academia Sinica/National Chao Tung University(その他の国・地域  台湾)

    • Related Report
      2018 Annual Research Report
  • [Journal Article] Strong Fermi Resonance Associated with Proton Motions Revealed by Vibrational Spectra of Asymmetric Proton-Bound Dimers2021

    • Author(s)
      Qian-Rui Huang, Ryunosuke Shishido, Chih-Kai Lin, Chen-Wei Tsai, Jake A. Tan, Asuka Fujii, Jer-Lai Kuo
    • Journal Title

      Angewandte Chemie International Edition

      Volume: 60 Issue: 4 Pages: 1936-1941

    • DOI

      10.1002/anie.202012665

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Understanding Fermi resonances in the complex vibrational spectra of the methyl groups in methylamines2021

    • Author(s)
      Qian-Rui Huang, Tomoya Endo, Saurabh Mishra, Bingbing Zhang, Li-Wei Chen, Asuka Fujii, Ling Jiang, G. Naresh Patwari, Yoshiyuki Matsuda, Jer-Lai Kuo
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 23 Issue: 6 Pages: 3739-3747

    • DOI

      10.1039/d0cp05745b

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Anharmonic Coupling Revealed by the Vibrational Spectra of Solvated Protonated Methanol: Fermi Resonance, Combination Bands, and Isotope Effect2021

    • Author(s)
      Chih-Kai Lin, Qian-Rui Huang, Ying-Cheng Li, Ha-Quyen Nguyen, Jer-Lai Kuo, Asuka Fujii
    • Journal Title

      The Journal of Physical Chemistry A

      Volume: 125 Issue: 9 Pages: 1910-1918

    • DOI

      10.1021/acs.jpca.1c00068

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Migrations and Catalytic Action of Water Molecules in the Ionized Formamide-(H2O)2 Cluster2020

    • Author(s)
      Yoshiyuki Matsuda, Yutaro Hirano, Shinichi Mizutani, Daichi Sakai, Asuka Fujii, Satoshi Maeda, Koichi Ohno
    • Journal Title

      The Journal of Physical Chemistry A

      Volume: 124 Issue: 14 Pages: 2802-2807

    • DOI

      10.1021/acs.jpca.0c00637

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Effects of mixing between short-chain and branched-chain alcohols in protonated clusters2020

    • Author(s)
      Po-Jen Hsu, Takahiro Shinkai, Pei-Han Tai, Asuka Fujii, Jer-Lai Kuo
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 22 Issue: 23 Pages: 13223-13239

    • DOI

      10.1039/d0cp01116a

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Infrared spectroscopic observation of the McLafferty rearrangement in ionized 2-pentanone2020

    • Author(s)
      Ryo Yasumoto, Yoshiyuki Matsuda, Asuka Fujii
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 22 Issue: 34 Pages: 19230-19237

    • DOI

      10.1039/d0cp02602f

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Vibrational spectroscopy of protonated amine-water clusters: tuning Fermi resonance and lighting up dark states2020

    • Author(s)
      Chih-Kai Lin, Ryunosuke Shishido, Qian-Rui Huang, Asuka Fujii, Jer-Lai Kuo
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 22 Issue: 38 Pages: 22035-22046

    • DOI

      10.1039/d0cp03229h

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Vibrational Coupling in Solvated H3O+: Interplay between Fermi Resonance and Combination Band2020

    • Author(s)
      Qian-Rui Huang, Ying-Cheng Li, Tomoki Nishigori, Marusu Katada, Asuka Fujii, Jer-Lai Kuo
    • Journal Title

      The Journal of Physical Chemistry Letters

      Volume: 11 Issue: 23 Pages: 10067-10072

    • DOI

      10.1021/acs.jpclett.0c03059

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] IR Spectroscopic Investigation on Isomerization of Ionized Ethylene Glycol2019

    • Author(s)
      Yoshiyuki Matsuda, Ayumu Matsuura, Takahiro Kamiyama, Asuka Fujii
    • Journal Title

      J. Phys. Chem. A

      Volume: 123 Issue: 24 Pages: 5122-5128

    • DOI

      10.1021/acs.jpca.9b02591

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Influence of the microsolvation on hemibonded and protonated hydrogen sulfide: infrared spectroscopy of [(H2S)n(X)1]+ and H+(H2S)n(X)1 (n = 1 and 2, X = water, methanol, and ethanol)2019

    • Author(s)
      Keigo Hattori, Dandan Wang, Asuka Fujii
    • Journal Title

      Phys.Chem.Chem.Phys.

      Volume: 21 Issue: 29 Pages: 16064-16074

    • DOI

      10.1039/c9cp03159f

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Effects of solvent molecules on hemi-bonded (CH3SH)2 +: infrared absorption of [(CH3SH)2-X]+ with X = H2O, (CH3)2CO, or NH3 and (CH3SH)n + (n = 3-6)2019

    • Author(s)
      Min Xie, Huei-Ru Tsai, Asuka Fujii, Yuan-Pern Lee
    • Journal Title

      Phys.Chem.Chem.Phys.

      Volume: 21 Issue: 29 Pages: 16055-16063

    • DOI

      10.1039/c9cp03158h

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Infrared Spectroscopic Study on Trimethyl Amine Radical Cation: Correlation between Proton-Donating Ability and Structural Deformation2019

    • Author(s)
      Tomoya Endo, Yoshiyuki Matsuda, Shohei Moriyama, Asuka Fujii
    • Journal Title

      J. Phys. Chem. A

      Volume: 123 Issue: 28 Pages: 5945-5950

    • DOI

      10.1021/acs.jpca.9b01261

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] The S-pi hemibond and its competition with the S-S hemibond in the simplest model system: infrared spectroscopy of the [benzene-(H2S)n]+ (n = 1–4) radical cation clusters2019

    • Author(s)
      Dandan Wang, Keigo Hattori, Asuka Fujii
    • Journal Title

      Chem. Sci.

      Volume: 10 Issue: 30 Pages: 7260-7268

    • DOI

      10.1039/c9sc02476j

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Electronic and Infrared Spectroscopy of Benzene-(H2S)n (n = 1 and 2): The Prototype of the SH-π Interaction2019

    • Author(s)
      Dandan Wang, Pragya Chopra, Sanjay Wategaonkar, Asuka Fujii
    • Journal Title

      J. Phys. Chem. A

      Volume: 123 Issue: 33 Pages: 7255-7260

    • DOI

      10.1021/acs.jpca.9b02199

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Spectral Characterization of Three-Electron Two-Center (3e-2c) Bonds of Gaseous CH3S∴S(H)CH3 and (CH3SH)2 + and Enhancement of the 3e-2c Bond upon Protonation2018

    • Author(s)
      Min Xie, Zhitao Shen, Dandan Wang, Asuka Fujii, Yuan-Pern Lee
    • Journal Title

      J. Phys. Chem. Lett.

      Volume: 9 Issue: 13 Pages: 3725-3730

    • DOI

      10.1021/acs.jpclett.8b01491

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Infrared Spectroscopy of Protonated Phenol-Water Clusters2018

    • Author(s)
      Marusu Katada, Asuka Fujii
    • Journal Title

      J. Phys. Chem. A

      Volume: 122 Issue: 27 Pages: 5822-5831

    • DOI

      10.1021/acs.jpca.8b04446

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Hydrogen bond network structures of protonated short-chain alcohol clusters2018

    • Author(s)
      Asuka Fujii, Natsuko Sugawara, Po-Jen Hsu, Takuto Shimamori, Ying-Cheng Li, Toru Hamashima, Jer-Lai Kuo
    • Journal Title

      Phys. Chem. Chem. Phys.

      Volume: 20 Issue: 22 Pages: 14971-14991

    • DOI

      10.1039/c7cp08072g

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Competition between hydrogen bonds and van der Waals forces in intermolecular structure formation of protonated branched-chain alcohol clusters2018

    • Author(s)
      Natsuko Sugawara, Po-Jen Hsu, Asuka Fujii, Jer-Lai Kuo
    • Journal Title

      Phys. Chem. Chem. Phys.

      Volume: 20 Issue: 39 Pages: 25482-25494

    • DOI

      10.1039/c8cp05222k

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Presentation] プロトン付加アルコールクラスターの水素結合に対するフッ素置換効果の赤外分光研究2020

    • Author(s)
      新海孝洋、藤井朱鳥、Po-Jen Hsu、Jer-Lai Kuo
    • Organizer
      分子科学会オンライン討論会
    • Related Report
      2020 Annual Research Report
  • [Presentation] アルカン2量体正イオンにおける水素分子脱離前駆体の赤外分光研究:分子間H-H準共有結合の形成2020

    • Author(s)
      安本 凌、松田欣之、藤井朱鳥
    • Organizer
      分子科学会オンライン討論会
    • Related Report
      2020 Annual Research Report
  • [Presentation] Infrared spectroscopy of hemibonded clusters of H2S2019

    • Author(s)
      Asuka Fujii
    • Organizer
      ACS Spring 2019 National Meeting
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Infrared spectroscopy of [(H2S)2(X)1]+ (X=water, methanol, ethanol): Influence of the microsolvation on the hemibond2019

    • Author(s)
      Keigo Hattori, Dandan Wang, Asuka Fujii
    • Organizer
      74th International symposium on molecular spectroscopy
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 2-ピリドン2量体負イオン内のプロトン移動反応に対する水和による抑制効果2019

    • Author(s)
      前山俊彦、藤井朱鳥
    • Organizer
      第13回分子科学討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] ホルムアミド-(H2O)3のイオン化誘起異性化反応の赤外分光研究2019

    • Author(s)
      松田欣之、平野裕太郎、藤井朱鳥
    • Organizer
      第13回分子科学討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] 赤外分光によるペンタノンイオンにおけるマクラファティ転位の観測2019

    • Author(s)
      安本凌、松田欣之、藤井朱鳥
    • Organizer
      第13回分子科学討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] プロトン付加及びラジカル正イオン硫化水素クラスターに対する溶媒和の影響2019

    • Author(s)
      服部圭吾、王丹丹、藤井朱鳥
    • Organizer
      第13回分子科学討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] S-半結合の観測:[benzene-(H2S)n]+ (n=1-4)の赤外分光2019

    • Author(s)
      王丹丹、服部圭吾、藤井朱鳥
    • Organizer
      第13回分子科学討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Infrared spectroscopy of intermediate in the McLafferty rearrangement of ionized pentanone2019

    • Author(s)
      安本凌、松田欣之、藤井朱鳥
    • Organizer
      2019年度化学系学協会東北大会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Infrared spectroscopy of protonated alcohol clusters: Competition and cooperation among hydrogen bond, dispersion, and steric hindrance2019

    • Author(s)
      Asuka Fujii
    • Organizer
      WRHI International Workshop on Advanced laser Spectroscopy for Soft Molecular Systems
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Protonated methanol-water mixed clusters: Hydrogen bond structures and their temperature dependence2018

    • Author(s)
      Asuka Fujii
    • Organizer
      The 8th cross strait workshop on chemical dynamics and kinetics
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] エチレングリコールのイオン化後続過程の赤外分光研究2018

    • Author(s)
      松田欣之、松浦歩、神山貴大、藤井朱鳥
    • Organizer
      第12回分子科学討論会
    • Related Report
      2018 Annual Research Report
  • [Presentation] 水和(2-ピリドン/2-ヒドロキシピリジン)2量体負イオンの光電子分光2018

    • Author(s)
      前山俊彦、藤井朱鳥
    • Organizer
      第12回分子科学討論会
    • Related Report
      2018 Annual Research Report
  • [Presentation] ベンゼン-(H2S)nクラスターのレーザー分光研究2018

    • Author(s)
      王丹丹、藤井朱鳥
    • Organizer
      第12回分子科学討論会
    • Related Report
      2018 Annual Research Report
  • [Presentation] H+(H2S)n(H2O)1の赤外分光 ~混合クラスターにおける余剰プロトンの位置決定~2018

    • Author(s)
      服部圭吾、王丹丹、藤井朱鳥
    • Organizer
      第12回分子科学討論会
    • Related Report
      2018 Annual Research Report
  • [Presentation] Infrared spectroscopy of hemibonded clusters of H2S2018

    • Author(s)
      Asuka Fujii
    • Organizer
      WRHI international workshop: Advanced laser spectroscopy of soft molecular systems
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Infrared spectroscopy of hemibonded clusters of H2S2018

    • Author(s)
      Asuka Fujii
    • Organizer
      10th Asian Photochemistry Conference
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Remarks] 東北大学 大学院理学研究科化学専攻 量子化学研究室

    • URL

      http://web.tohoku.ac.jp/qclab/

    • Related Report
      2020 Annual Research Report

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Published: 2018-04-23   Modified: 2022-08-19  

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