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High density collection of molecular ion clusters and their photoexcitation dynamics

Research Project

Project/Area Number 07454190
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field 機能・物性・材料
Research InstitutionOkazaki National Research Institutes (1996-1997)
Kyushu University (1995)

Principal Investigator

NISHI Nobuyuki  OKAZAKI NATIONAL RESEARCH INSTITUTE,Institute for Molecular Science, Professor, 分子科学研究所, 教授 (60013538)

Co-Investigator(Kenkyū-buntansha) OHASHI Kazuhiko  OKAZAKI NATIONAL RESEARCH INSTITUTE,Institute for Molecular Science, Research As, 分子科学研究所, 助手 (80213825)
Project Period (FY) 1995 – 1997
Project Status Completed (Fiscal Year 1997)
Budget Amount *help
¥7,800,000 (Direct Cost: ¥7,800,000)
Fiscal Year 1997: ¥200,000 (Direct Cost: ¥200,000)
Fiscal Year 1996: ¥3,600,000 (Direct Cost: ¥3,600,000)
Fiscal Year 1995: ¥4,000,000 (Direct Cost: ¥4,000,000)
Keywordsmolecular ion clusters / matrix isolation / charge hopping / photodissociation / IR spectroscopy / benzene cation / 赤外分光 / 分子イオン / クラスター / ソフトランディング / 分子分光
Research Abstract

In order to study electronic states and dynamics of highly condensed molecular ion clusters, we designed a molecular beam apparatus with a soft-landing ion deosition and IR and UVabsorption spectrometers. A molecular beam generated from liquid droplets by adiabatic Big-Bang explosion is directly injected against 10-inch diffusion pump. Ions are extracted perpendicular to the beam axis, mass-selected, decelerated, and gently imbedded in a rare gas matrix. As atest experiment, benzene cations are deposited in argon matrices at 4 K.Contamination of the background neutral benzene was so little that after 10 hour deposition we can detect the neutrals by UV absorption spectrometry. The electronic spectrum of benzene cation showed that the electronic orbitals of argon atoms around the cation is highly distorted and polarized by the cation. The high dnsity deposition process was accompanied with a big difficulty without any codeposition of negative ions. Frequent explosive ablation of the new surface layrs was observed during the deposition. It is necessary to design a natural negative ion deposition mechanism in a chamber.
We also observed a charge hopping phenomenon in benzene trimer cations after vibrational excitation of a C-H stretching motion of an ionic molecule. The excitation of an isotopic mixture (C_6H_6) ^+ (C_6D_6)_2 resulted in the fragmentation yielding (C_6D_6)_2^+ and [ (C_6D_6) (C_6H_6) ]^+ with a ratio of 1 : 2. This is a statistical limit suggesting the hopping occurs sufficiently faster than the dissociation process. The observed line-widths of the C-H stretching bands showed sectral shifts dependent on the position of the charged molecules in the cluster and also on the masses of the neighboring molecules. Rather broad line-widths indicates that the relaxation is of the order of 100-150fs.

Report

(4 results)
  • 1997 Annual Research Report   Final Research Report Summary
  • 1996 Annual Research Report
  • 1995 Annual Research Report
  • Research Products

    (31 results)

All Other

All Publications (31 results)

  • [Publications] 井口 佳哉: "Formation of benzene dimer cations in neat liquid benzene studied by femtosecond transient absortion spectroscopy" Chemical Physics Letterts. 269. 298-304 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] 松本 正樹: "Charge Delocalization in Benzene-Naphthalene Hetero-Dimer Cation" Journal of Physical Chemistry. 101. 4574-4578 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] 中井 泰弘: Electronic structures and photoevaporation dynamics of benzene cluster ions.

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] 市村 禎二郎: "Photofragmentation of Chlorotoluenes and Dichlorobenzenes:Substituent effects on the dissociation mechanism,.." Journal of Chemical Physics. 107. 73-78 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] 井口 佳哉: "Infrared photodissociation spectroscopy of benzene trimer ions.Switching of the dimer ion core in vibrationally excited states" Journal of Physical Chemistry. 101. 472-480 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Kazuhiko Ohashi, Kei Adachi, and Nobuyuki Nishi: ""Unimolecular Dissociation Kinetics of Benzene Cluster Ions"" Bull.Chem.Soc.Jpn.69. 915-924 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Kazuhiko Ohashi, Yoshiya Inokuchi, and Nobuyuki Nishi: ""Photodissociation spectroscopy of phenol dimer ion : Lack of resonance interaction between the aromatic rings"" Chem.Phys.Lett. 257. 137-142 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Kazuhiko Ohashi and Nobuyuki Nishi: ""Spectroscopy and excited-state dynamics of benzene-timer ion"" Surface Review Letters. 3. 601-605 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Kazuhiko Ohashi, Yoshiya Inokuchi, and Nobuyuki Nishi: ""Pump-probe photodepletion spectroscopy of (C_6H_6) _2^+ : Identification of spectrum in the charge resonance band region"" Chem.Phys.Lett.263. 167-172 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Yoshiya Inokuchi, Masaki Matsumoto, Kazuhiko Ohashi, and Nobuyuki Nishi: ""Charge Resonance and Charge Transfer Interactins in Naphthalene Homo- and Hetero-Dimers"" Resonance Ionization spectroscopy American Institute of Physics. 231-236 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Yasuhiro Nakai, Kazuhiko Ohashi, and Nobuyuki Nishi: ""Electronic structures and photoevaporation dynamics of benzene cluster ions"" J.Phys. Chem.101. 472-480 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Yoshiya Inokuchi, Yukito Naitoh, Kazuhiko Ohashi, Ken-ichi Saitow, Keitaro Yoshihara, and Nobuyuki Nishi: ""Formation of benzene dimer cations in neat liuid benzene studied by femtosecond transient obsorption spectroscopy"" Chem.Phys.Lett.269. 298-304 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Masaki Matsumoto, Yoshiya Inokuchi, Kazuhiko Ohashi, and Nobuyuki Nishi: ""Charge Delocalization in Benzene-Naphthalene Hetero-Dimer Cation"" J.Phys.Chem.101. 4574-4578 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Teijiro Ichimura, Yuji Mori, Hisanori Shinohara, and Nobuyuki Nishi: ""Photofragmentation of Chlorotoluenes and Dichlorobenzenes : Substituent effects on the dissociation mechanism, and angular distibution of Cl fragment"" J.Chem.Phys.107. 835-842 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Yoshiya Inokuchi, Kazuhiko Ohashi, and Nobuyuki Nishi: ""Infrared photodissociation spectroscopy of benzene trimer ions. Switching of the dimer ion core in vibrationally excited states"" Chem.Phys.Lett.279. 73-78 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] 井口佳哉: "Formation of benzene dimer cations in neat liquid benzene studied by femtosecond transient absorption spectroscopy" Chemical Physics Letterts. 269. 298-304 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] 松本政樹: "Charge Delocalization in Benzene-Naphthalene Hetero-Dimer Cation" Journal of Physical Chemistry. 101. 4574-4578 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] 中井泰弘: "Electronic structures and photoevaporation dynamics of benzene cluster ions" Journal of Physical Chemistry. 101. 472-480 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] 市村禎二郎: "Photofragmentation of Chlorotoluenes and Dichlorobenzenes : Substituent effects on the dissociation mechanism,.." Journal of Chemical Physics. 107. 835-842 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] 井口佳哉: "Infrared photodissociation spectroscopy of benzene trimer ions. Switching of the dimer ion core in vibrationally excited states" Chemical Physics Letters. 279. 73-78 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] 大橋和彦: "Unimolecular dissociation kinetics of benzene cluster ions" Bulletin of Chemical Society of Japan. 69. 915-924 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] 大橋和彦: "Spectroscopy and excited-state dynamics of benzene-trimer ion" Surface Review Letters. 3. 601-605 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] 大橋和彦: "Photodissociation spectroscopy of phenol dimerion. Lack of resonance interaction between the aromatic rings" Chemical Physics Letters. 257. 137-142 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] 大橋和彦: "Pump-probe photodepletion spectroscopy of (C6H6) 2+. Identification of spectrum in the charge resonance band region" Chemical Physics Letters. 263. 167-172 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] 中井泰弘: "Electronic structures and photoevaporation dynamics of benzene cluster ions" Journal of Physical Chemistry. 101. 472-480 (1997)

    • Related Report
      1996 Annual Research Report
  • [Publications] 中井泰広: "“Photoinduced evaporation of benzene cluster ions"" Chemical Physics Letters. 233. 36-40 (1995)

    • Related Report
      1995 Annual Research Report
  • [Publications] 井口佳哉: "“Photodissociation spectrum of naphthalene dimer cation"" Journal of Physical Chemistry. 99. 3416-3418 (1995)

    • Related Report
      1995 Annual Research Report
  • [Publications] 大橋和彦: "“Photodissociation mechanism of benzene cluster ions on the excitation with hn=0.5-3.0eV"" Laser Chemistry. 15. 93-111 (1995)

    • Related Report
      1995 Annual Research Report
  • [Publications] 松本政樹: "“Structure of Clesters in Ethanol-Water Binary Solutions Studied by Mass Spectrometry and X-Ray Diffraction"" Bulletin of Chemical Society of Japan. 68. 1775-1783 (1995)

    • Related Report
      1995 Annual Research Report
  • [Publications] 脇坂昭彦: "“Preferential Solvation controlled by Clustering Conditions of Acetonitrile-Water Mixtures"" Journal of Chemical Society, Faraday Transaction. 91. 4063-4069 (1995)

    • Related Report
      1995 Annual Research Report
  • [Publications] 西信之: "Hydrogen Bonding Cluster Formation and Hydrophobic Solute Association in Aqueous Solution of Ethanol" Journal of Physical Chemistry. 99. 462-468 (1995)

    • Related Report
      1995 Annual Research Report

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Published: 1995-04-01   Modified: 2016-04-21  

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