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Dynamics of Gas-Phase Clusters as Studied by Tune-Resolved Photoelectron

Research Project

Project/Area Number 09440210
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field Physical chemistry
Research InstitutionThe University of Tokyo (1998-1999)
Okazaki National Research Institutes (1997)

Principal Investigator

NAGATA Takashi  Graduate School of Arts and Sciences, The University of Tokyo, Professor, 大学院・総合文化研究科, 教授 (10164211)

Co-Investigator(Kenkyū-buntansha) ZHU LEI  Okazaki National Research Institute, The Institute of Molecular Science, Research assistant, 分子科学研究所, 助手
TSUKUDA TATSUYA  Graduate School of Arts and Sciences, The University of Tokyo, Research assistant, 大学院・総合文化研究科, 助手 (90262104)
Project Period (FY) 1997 – 1999
Project Status Completed (Fiscal Year 1999)
Budget Amount *help
¥11,700,000 (Direct Cost: ¥11,700,000)
Fiscal Year 1999: ¥2,100,000 (Direct Cost: ¥2,100,000)
Fiscal Year 1998: ¥3,300,000 (Direct Cost: ¥3,300,000)
Fiscal Year 1997: ¥6,300,000 (Direct Cost: ¥6,300,000)
KeywordsMolecular cluster anions / Photoelectron spectroscopy / Energy dissipation / Electronic isomer / Structural fluctuation / Tri-iodide anion / Solvent effects / Microsolvation
Research Abstract

One of the fundamental issues regarding the properties of clusters, aggregates of atoms or molecules in the gas phase, concerns the dynamics of energy dissipation among their enormous numbers of degrees of freedom. In the present study, we have investigated (1) the energy relaxation processes, (2) the isomerization processes and (3) photodissociation processes of negatively-charged molecular clusters in terms of their geometrical and electronic structures. The findings are summarized as follows :
1. The time evolution of the photoelectron signal from an electronically-excited (CィイD26ィエD2FィイD26ィエD2)ィイD2nィエD2ィイD1-ィエD1 is probed by fs time-resolved photoelectron spectroscopy. The excited state is found to decay with a lifetime of 1.5 ps, which can be regarded as the time required for the energy disposal into a specific intermolecular vibrational mode in the cluster anions.
2. The electronic structures of (C0ィイD22ィエD2)ィイD2nィエD2ィイD1-ィエD1, (CSィイD22ィエD2)ィイD2nィエD2ィイD1-ィエD1 and [(C0ィイD22ィエD2)ィイD2 … More nィエD2ROH]ィイD1-ィエD1 (R = H, CHィイD23ィエD2) are investigated by photoelectron spectroscopy combined with ab initio calculations, demonstrating the coexistence of isomers having different electronic structures. These "electronic isomers" are well described as [CィイD22ィエD2OィイD24ィエD2ィイD1-ィエD1・ROH(COィイD22ィエD2)ィイD2n-2ィエD2] and [C0ィイD22ィエD2ィイD1-ィエD1・ROH (COィイD22ィエD2)ィイD2n-1ィエD2]
3. The photodepletion-photoelectron measurement has revealed the floppiness of the isomeric forms of [(C0ィイD22ィエD2) ィイD24ィエD2HィイD22ィエD2O]ィイD1-ィエD1 clusters : the cluster anions are fluctuating between two forms of isomers as [CィイD22ィエD2OィイD24ィエD2ィイD1-ィエD1・HィイD22ィエD2O (C0ィイD22ィエD2) ィイD22ィエD2] 【double arrow】 [C0ィイD22ィエD2ィイD1-ィエD1・HィイD22ィエD20(C0ィイD22ィエD2) ィイD23ィエD2] at their own temperatures.
4. The photodissociation processes of gas-phase tri-iodide anion, IィイD23ィエD2ィイD1-ィエD1, along with its weakly bound clusters, IィイD23ィエD2ィイD1-ィエD1・M, are studied by a combination of an ion-beam technique with a time-of-flight (TOF) method. The experimental results obtained shows convincingly that a single solvent molecule can inhibit the more energy-demanding channel of the IィイD23ィエD2ィイD1-ィエD1 photofragmentation to a considerable extent, which opens up a possibility of controlling the IィイD23ィエD2ィイD1-ィエD1 photofragmentation process via stepwise microsolvation. Less

Report

(4 results)
  • 1999 Annual Research Report   Final Research Report Summary
  • 1998 Annual Research Report
  • 1997 Annual Research Report
  • Research Products

    (25 results)

All Other

All Publications (25 results)

  • [Publications] T. Tsukuda et al.: "Photoelectron Spectroscopy of (<@D22@>D2)<@D2n@>D2 Revisited: Core Switching in the 2 <= n <= 16 range."Chemical Physics Letters. 268. 429-433 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] T. Tsukuda et al.: "Reaction of Negatively -Charged Clusters of Carbon Dioxide with CH<@D23@>D2I : Formation of Novel Molecular Anion CH<@D23@>D2<@D22@>D2I<@D1-@>D1"Journal of Physical Chemistry. 101. 5103-5110 (1977)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] T. Tsukuda et al.: "Negative-Ion Photoelectron Spectroscopy of (CS<@D22@>D2)<@D2n@>D2<@D1-@>D1 as Studied by Photoelectron Spectroscopy"Chemical Physics Letters. 279. 179-184 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] T. Tsukuda et al.: "Electronic Structures of (SO<@D22@>D2)<@D2n@>D2<@D1-@>D1as Studied by Photoelectron Spectroscopy"International Journal of Mass Spectrometry and Icon Processes. 171. 273-280 (1977)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] M. Saeki et al.: "Photoabsorption and Photofragmentation Studies of Acetyloxy lodide Anion CH<@D23@>D2<@D22@>D2I<@D1-@>D1"Chemical Physics Letters. 280. 348-352 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] T.Tsukuda et al.: "Formation of N<@D23@>D2O<@D1-@>D1<@D23@>D2 Anion in (NO)<@D1-@>D1<@D2n@>D2: Photoelectron spectroscopy and Ab initio calculations"Chemical Physics Letters. 295. 416-422 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] T. Tsukuda et al.: "Electronic Isomers in [(<@D22@>D2)<@D2n@>D2ROH]<@D1-@>D1 Cluster Anions. I. Photoelectron Spectroscopy."Journal of Chemical Physics. 110. 7846-7857 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] M. Saeki et al.: "Electronic Isomers in [(<@D22@>D2)<@D2n@>D2ROH]<@D1-@>D1 Cluster Anions. II. Ab initio Calculations."Journal of Chemical Physics. 111. 6333-6344 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] T. Tsukuda, M. A. Johnson and T. Nagata: "Photoelectron Spectroscopy of (C0ィイD22ィエD2)ィイD2nィエD2ィイD1-ィエD1 Revisited : Core Switching in the 2 ≦ n ≦ 16 range."Chemical Physics Letters. 268. 429-433 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] T. Tsukuda, M. Saeki, S. Iwata and T. Nagate: "Reaction of Negatively-Charged Clusters of Carbon Dioxide with CHィイD23ィエD2I : Formation of Novel Molecular Anion CHィイD23ィエD2C0ィイD22ィエD2IィイD1-ィエD1."Journal of Physical Chemistry. 101. 5103-5110 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] T. Tsukuda, T. Hirose and T. Nagata: "Negative-Ion Photoelectron Spectroscopy of (CSィイD22ィエD2)ィイD2nィエD2ィイD1-ィエD1 : Coexistence of Electronic Isomers."Chemical Physics Letters. 279. 179-184 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] T. Tsukuda, T. Hirose and T. Nagata: "Electronic Structures of (SOィイD22ィエD2)ィイD2nィエD2ィイD1-ィエD1 as Studied by Photoelectron Spectroscopy."International Journal of Mass Spectrometry and Ion Processes. 171. 273-280 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] M. Saeki, L. Zhu, T. Tsukuda, S. Iwata and T. Nagata: "Photoabsorption and Photofragmentation Studies of Acetyloxy Iodide Anion CHィイD2dィエD2COィイD22ィエD2IィイD1-ィエD1."Chemical Physics Letters. 280. 348-352 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] T. Tsukuda, M. Saeki, L. Zhu and T. Nagata: "Formation of NィイD23ィエD2OィイD23ィエD2ィイD1-ィエD1 Anion in (NO)ィイD2nィエD2ィイD1-ィエD1 : Photoelectron spectroscopy and Ab initio calculations."Chemical Physics Letters. 295. 416-422 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] T. Tsukuda, M. Saeki, R. Kimura and T. Nagata: "Electronic Isomers in [(C0ィイD22ィエD2)ィイD2nィエD2ROH]ィイD1-ィエD1 Cluster Anions. I. Photoelectron Spectroscopy."Journal of Chemical Physics. 110. 7846-7857 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] M. Saeki, T. Tsukuda, S. Iwata and T. Nagata: "Electronic Isomers in [(C0ィイD22ィエD2)ィイD2nィエD2ROH]ィイD1-ィエD1 Cluster Anions. II. Ab initio Calculations."Journal of Chemical Physics. 111. 6333-6344 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] T. Tsukuda et al.: "Electronic isomers in 〔(CO_2)_nROH]^- cluster anions. I.Photoelectron spectroscopy."Journal of Chemical Physics. 110. 7846-7857 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] M. Saeki et al.: "Electronic isomers in 〔(CO_2)_nROH]^- cluster anions. II. Ab initio calculations."Journal of Chemical Physics. 111. 6333-6344 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] T.Tsukuda et al.: "Formation of N_3O_3 anion in (NO)n^- : Photoelectron spectroscopy and ab initio calculations." Chemical Physics Letters. 295. 416-422 (1988)

    • Related Report
      1998 Annual Research Report
  • [Publications] T.Tsukuda et al.: "Electronic isomers in 〔(CO_2)_nROH〕^-cluster anions.I.Photoelectron spectroscopy." Journal of Chemical Physics. (印刷中). (1999)

    • Related Report
      1998 Annual Research Report
  • [Publications] T.Tsukuda et al.: "Photoelectron Spectroscopy of (CO_2)_n^- Revisited : Core Switching in the 2≦n≦16range" Chemical Physics Letters. 268. 429-433 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] T.Tsukuda et al.: "Reaction of Negatively-Charged Clusters of Carbon Dioxide with CH_3I : Formation of Novel Molecular Anion CH_3CO_2I^-" Journal of Physical Chemistry. 101. 5103-5110 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] T.Tsukuda et al.: "Negative-Ion Photoelectron Spectroscopy of (CS_2)_n^- : Coexistence of Electronic Isomers" Chemical Physics Letters. 279. 179-184 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] M.Saeki et al.: "Photoabsorption and Photofragmentation Studies of Acetyloxy Iodide Anion CH_3CO_2I^-" Chemical Physics Letters. 280. 348-352 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] T.Tsukuda et al.: "Electronic Structures of (SO_2)_n^- as Studied by Photoelectron Spectroscopy" International Journal of Mass Spectrometry and Ion Processes. (印刷中). (1997)

    • Related Report
      1997 Annual Research Report

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Published: 1997-04-01   Modified: 2016-04-21  

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