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Structural Properties of Gas-Phase Solvated Electrons and Anions-Toward the Microscopic Understanding of Stabilization Mechanism-

Research Project

Project/Area Number 18550007
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeSingle-year Grants
Section一般
Research Field Physical chemistry
Research InstitutionThe University of Tokyo

Principal Investigator

NAGATA Takashi  The University of Tokyo, Graduate School of Arts and Sciences, Professor (10164211)

Project Period (FY) 2006 – 2007
Project Status Completed (Fiscal Year 2007)
Budget Amount *help
¥4,020,000 (Direct Cost: ¥3,600,000、Indirect Cost: ¥420,000)
Fiscal Year 2007: ¥1,820,000 (Direct Cost: ¥1,400,000、Indirect Cost: ¥420,000)
Fiscal Year 2006: ¥2,200,000 (Direct Cost: ¥2,200,000)
Keywordscluster / hydrated electron / valence anion / hydrogen-bonding network / photoelectron spectroscopy / IR photodissociation spectroscopy / 溶媒和電子
Research Abstract

The aim of the present research project was to attain a microscopic understanding of the stabilization mechanism at play in solvated electrons and anions through the systematic study about the electronic properties of gas-phase cluster anions in heterogeneous solvation environments.
1. Reconstruction of the hydrogen-bonding network in (H_2O)_n^-: We demonstrated that the incorporation of a single D_2O or CH_3OH into (H_2O)_<6,7>^-proceeded efficiently without losing any H_2O constituent, by exploiting the "Ar-mediated" process such as (H_2O)_n^-Ar_m+M→[M・(H_2O)_n^-Ar_m]^†→[(H_2O)_nM]^-+mAr. The photoelectron spectroscopic measurements revealed that isomeric interconversion occurred in [(H_2O)_nM]^-through an extensive reconstruction of the hydrogen-bonding network during the incorporation processes.
2. Formation and photodestruction of dual dipole-bound anion: A new type of dipole-bound anion composed of water and a polar molecule with μ>2.8 D was generated by the incorporation reaction … More of argon-solvated water hexamer anions, (H_2O)_6^-Ar_m. The newly-found anion can be regarded as a dual dipole-bound species described as (H_2O)_6{e^-} M, where the diffuse excess electron interacts with both (H_2O)_6 and M via the individual electron-dipole interaction. The dual dipole-bound anion also serves as a precursor to the hydrated valence anion of M.
3. Structures of [(CO_2)_n(ROH)_m]^-(R=H, CH_3) cluster anions: The solvation structures of [(CO_2)_n(ROH)_m]^-were investigated by infrared photodissociation spectroscopy combined with ab initio calculations. A significant entrainer effect was observed such that the incorporated protic molecule stabilizes CO_2 effectively through the single ionic hydrogen-bonding interaction.
4. Valence anions stabilized by surrounding multi-dipoles: The electronic properties of the negatively-charged clusters of acetone and water molecules, [(Me_2CO)_n(H_2O)_m]^-, were studied by photoelectron imaging spectroscopy. The measurement indicates possibility that a new type of stabilization mechanism is operative in [(Me_2CO)_n(H_2O)_m]^-: i. e., the valence anion of Me_2CO is stabilized by an electrostatic field generated by the surrounding multi-dipoles. Less

Report

(3 results)
  • 2007 Annual Research Report   Final Research Report Summary
  • 2006 Annual Research Report
  • Research Products

    (41 results)

All 2008 2007 2006

All Journal Article (17 results) (of which Peer Reviewed: 9 results) Presentation (24 results)

  • [Journal Article] Structures of[(CO_2)_n(CH_3OH)_m]^-(n=1-4, m=1, 2)cluster anions.2008

    • Author(s)
      A. Muraoka
    • Journal Title

      Journal of Physical Chemistry A112

      Pages: 4906-4913

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Structures of C_2S_4^-molecular anion : Photoelectron spectroscopy and theoretical calculations.2008

    • Author(s)
      Y. Matsuyama
    • Journal Title

      Chemical Physics Letters 457

      Pages: 31-35

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] An IR study of (CO_2)^+_n(n=3-8)cluster ions in the 1000-3800 cm^<-1> region.2008

    • Author(s)
      Y. Inokuchi
    • Journal Title

      Journal of Chemical Physics 128

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Structures of [(CO_2)_n(CH_3OH)_m]^- (n = 1 -4, m = 1, 2) cluster anions.2008

    • Author(s)
      A. Muraoka, Y. Inokuchi, T. Nagata
    • Journal Title

      Journal Physical Chemistry A112

      Pages: 4906-4913

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Journal Article] Structures of C_2S_4^- molecular anion : Photoelectron spectroscopy and theoretical calculations.2008

    • Author(s)
      Y. Matsuyama, T. Nagata
    • Journal Title

      Chemical Physics Letters 457

      Pages: 31-35

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Journal Article] An IR study of (CO_2)_n^+ (n = 3 - 8) cluster ions in the 1000 - 3800 cm^<-1> region.2008

    • Author(s)
      Y. Inokuchi, A. Muraoka, T. Nagata, T. Ebata
    • Journal Title

      Journal Chemical Physics 129

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Journal Article] Structures of C_2S_4<-> molecular anion: photoelectron spectroscopy and theoretical calculations.2008

    • Author(s)
      Y. Matsuyama
    • Journal Title

      Chemical Physics Letter (掲載確定印刷定)

    • Related Report
      2007 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Structures of [(CO_2)_n(CH_3OH)_m]<-> (n=1-4,m=1,2)cluster anions.2008

    • Author(s)
      A. Muraoka
    • Journal Title

      Journal of Physical Chemistry A (掲載確定印刷定)

    • Related Report
      2007 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Photodissociation of gas-phase I_3^- : Comprehensive understanding of nonadiabatic dissociation dynamics.2007

    • Author(s)
      R. Nakanishi
    • Journal Title

      Journal of Chemical Physics 126

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Photodissociation of gas-phase I_3^- : Comprehensive understanding of nonadiabatic dissociation dynamics.2007

    • Author(s)
      R. Nakanishi, N. Saitou, T. Ohno, S. Kowashi, S. Yabushita, T. Nagata
    • Journal Title

      Journal Chemical Physics 126

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Journal Article] Photodissociation of gas-phase I_3<->: Comprehensive understanding of nonadiabatic dissociation dynamics.2007

    • Author(s)
      R. Nakanishi
    • Journal Title

      Journal of Chemical Physics 126

    • Related Report
      2007 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Photoelectron spectroscopy of acetone cluster anions, [(CH_3)_2CO]_n^-(n=2, 5-15).2006

    • Author(s)
      R. Nakanishi
    • Journal Title

      Chemical Physics Letters 427

      Pages: 56-61

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Formation of O_2CNO^-in the reaction of(CO_2)_n^- with NO.2006

    • Author(s)
      K. Sudoh
    • Journal Title

      Chemical Physics Letters 433

      Pages: 10-14

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Photoelectron spectroscopy of acetone cluster anions, [(CH_3)_2CO]_n^-(n = 2, 5 -15).2006

    • Author(s)
      R. Nakanishi, A. Muraoka, T. Nagata
    • Journal Title

      Chemical Physics Letters 427

      Pages: 56-61

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Journal Article] Formation of O_2CNO^- in the reaction of (CO_2)_n^-with NO.2006

    • Author(s)
      K. Sudoh, Y. Matsuyama, A. Muraoka, R. Nakanishi, T. Nagata
    • Journal Title

      Chemical Physics Letters 433

      Pages: 10-14

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Journal Article] Photoelectron spectroscopy of acetone cluster anions, 〔(CH_3)_2CO〕_n^-(n=2,5-15).2006

    • Author(s)
      R.Nakanishi, et al.
    • Journal Title

      Chemical Physics Letters 427

      Pages: 56-61

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Formation of O_2CNO^-in the reaction (CO_2)_n^- of with NO.2006

    • Author(s)
      K.Sudoh, et al.
    • Journal Title

      Chemical Pjysics Letters 433

      Pages: 10-14

    • Related Report
      2006 Annual Research Report
  • [Presentation] SO_2/O_2系から生成したSO_4^-の構造2008

    • Author(s)
      座間小百合
    • Organizer
      分子構造総合討論会2008
    • Place of Presentation
      福岡
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] 水和電子クラスター(H_2O)_n^-の分子取込み反応 : 原子価負イオン生成vsネットワーク構造転移2008

    • Author(s)
      中西隆造
    • Organizer
      分子構造総合討論会2008
    • Place of Presentation
      福岡
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] 赤外光解離分光法による, CO_2およびCS_2クラスターイオンの構造の解明2008

    • Author(s)
      井口佳哉
    • Organizer
      分子構造総合討論会2008
    • Place of Presentation
      福岡
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Formation of SO_4^- generated in the SO_2/O_2 systems.2008

    • Author(s)
      S. Zama, R. Nakanishi, A. Muraoka, M. Yamamoto, T. Nagata
    • Organizer
      Annual Meeting of Japan Society for Molecular Science
    • Place of Presentation
      Fukuoka
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Uptake reactions of (H_2O)_n^- : Formation of valence anion vs. network reconstruction.2008

    • Author(s)
      R. Nakanishi, T. Nagata
    • Organizer
      Annual Meeting of Japan Society for Molecular Science
    • Place of Presentation
      Fukuoka
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Photodissociation dynamics of gas-phase I_3^-.2008

    • Author(s)
      S. Kowashi, M. Sugawara, R. Nakanishi, T. Nagata, S. Yabushita
    • Organizer
      Annual Meeting of Japan Society for Molecular Science
    • Place of Presentation
      Fukuoka
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] IR photodissociation spectroscopy of cluster ions of CO_2 and CS_2.2008

    • Author(s)
      Y. Inokuchi, A. Muraoka, Y. Kobayashi, T. Nagata, T. Ebata
    • Organizer
      Annual Meeting of Japan Society for Molecular Science
    • Place of Presentation
      Fukuoka
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] I3^-光解離過程におけるミクロ溶媒効果2007

    • Author(s)
      加藤修吾
    • Organizer
      分子科学討論会2007
    • Place of Presentation
      仙台
    • Year and Date
      2007-09-20
    • Related Report
      2007 Annual Research Report
  • [Presentation] [(CO_2)_n(CH_3OH)_m]^-におけるイオン芯とメタノール分子の配位形態2007

    • Author(s)
      村岡 梓
    • Organizer
      分子科学討論会2007
    • Place of Presentation
      仙台
    • Year and Date
      2007-09-19
    • Related Report
      2007 Annual Research Report
  • [Presentation] (H_2O)_n^-のD_2O,CH_3OH付加反応による水素結合ネットワークの構造転移2007

    • Author(s)
      中西隆三
    • Organizer
      分子科学討論会2007
    • Place of Presentation
      仙台
    • Year and Date
      2007-09-18
    • Related Report
      2007 Annual Research Report
  • [Presentation] (H_2O)_n^-のD_2O, CH_3OH付加反応による水素結合ネットワークの構造転移2007

    • Author(s)
      中西隆造
    • Organizer
      分子構造総合討論会2007
    • Place of Presentation
      仙台
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] [(CO_2)_n, (CH_3OH)_m]^-におけるイオン芯とメタノール分子の配位形態2007

    • Author(s)
      村岡梓
    • Organizer
      分子構造総合討論会2007
    • Place of Presentation
      仙台
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] I_3^-光解離過程におけるミクロ溶媒効果2007

    • Author(s)
      加藤修吾
    • Organizer
      分子構造総合討論会2007
    • Place of Presentation
      仙台
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Reconstruction of the hydrogen-bonding networks of (H_2O)_n^- in the incorporation reactions with D_2O and CH_3OH2007

    • Author(s)
      R. Nakanishi, T. Nagata
    • Organizer
      Annual Meeting of Japan Society for Molecular Science
    • Place of Presentation
      Sendai
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Anionic cores and solvation mechanism in [(CO_2)_n(CH_3OH)_m]^-.2007

    • Author(s)
      A. Muraoka, Y. Inokuchi, T. Nagata
    • Organizer
      Annual Meeting of Japan Society for Molecular Science
    • Place of Presentation
      Sendai
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Microsolvation effects on the photodissociation dynamics of gas-phase I_3^-.2007

    • Author(s)
      S. Kato, R. Nakanishi, T. Nagata
    • Organizer
      Annual Meeting of Japan Society for Molecular Science
    • Place of Presentation
      Sendai
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] [(CO_2)_n(CH_3OH)_m]^-の異性体分布と溶媒和構造2006

    • Author(s)
      村岡梓
    • Organizer
      分子構造総合討論会2006
    • Place of Presentation
      静岡
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] (CO_2)_n^-を利用したC0_2^-ラジカル負イオンとNO, O_2の反応2006

    • Author(s)
      須藤虎太郎
    • Organizer
      分子構造総合討論会2006
    • Place of Presentation
      静岡
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] (H_2O)_n^-にクラスタ-と極性溶媒分子の反応-サイズ依存性と反応機構-2006

    • Author(s)
      中西隆造
    • Organizer
      分子構造総合討論会2006
    • Place of Presentation
      静岡
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] アセトンクラスター負イオンの光電子分光2006

    • Author(s)
      中西隆造
    • Organizer
      分子構造総合討論会2006
    • Place of Presentation
      静岡
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Solvation structures of [(CO_2)_n(CH_3OH)_m]^- isomers.2006

    • Author(s)
      A. Muraoka, Y. Inokuchi, T. Nagata
    • Organizer
      Annual Meeting of Japan Society for Molecular Science
    • Place of Presentation
      Shizuoka
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Reactions of CO_2^・- with NO and O_2 mediated by (CO_2)_n^- cluster anions.2006

    • Author(s)
      K. Sudoh, Y. Matsuyama, A. Muraoka, T. Nagata
    • Organizer
      Annual Meeting of Japan Society for Molecular Science
    • Place of Presentation
      Shizuoka
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Reactions of (H_2O)_n^- with polar molecules -Size-dependent reaction mechanism-2006

    • Author(s)
      R. Nakanishi, T. Nagata
    • Organizer
      Annual Meeting of Japan Society for Molecular Science
    • Place of Presentation
      Shizuoka
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Photoelectron spectroscopy of cluster anions of acetone.2006

    • Author(s)
      R. Nakanishi, A. Muraoka, T. Nagata
    • Organizer
      Annual Meeting of Japan Society for Molecular Science
    • Place of Presentation
      Shizuoka
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary

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Published: 2006-04-01   Modified: 2016-04-21  

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