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Real-time probing of Energy Dissipation Processes in Solvated Clusters

Research Project

Project/Area Number 08454177
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field Physical chemistry
Research InstitutionKyoto University

Principal Investigator

OHSHIMA Yasuhiro  Kyoto Univ., Graduate School of Science, Associate Professor, 大学院・理科研究科, 助教授 (60213708)

Project Period (FY) 1996 – 1997
Project Status Completed (Fiscal Year 1997)
Budget Amount *help
¥7,400,000 (Direct Cost: ¥7,400,000)
Fiscal Year 1997: ¥3,500,000 (Direct Cost: ¥3,500,000)
Fiscal Year 1996: ¥3,900,000 (Direct Cost: ¥3,900,000)
KeywordsClusters / ps Time-Resolved Spectroscopy / Solvation / Energy Dissipation / Laser-Induced Fluorescence / Charge-Transfer / Inter-System Crossing / 電子移動反応 / 系間交差
Research Abstract

The present research project aims to microscopic understanding on the energy dissipation processes in solvated clusters through ultrafast time-resolved measurements. Owing to the improvement in the experimental setup, such as the vacuum chambers and laser systems, the following results have been achieved.
1. The 1 : 1 cluster of 9,9'-bianthryl (BA) with water has been studied for detailed characterization of the twisted intramolecular charge transfer (TICT) reaction in BA.The torsional potential of BA in the cluster has been determined form the laser-induced-fluorescence observation of the torsional progressions. The potential in the cluster is much different from that in the monomer, indicating considerable modification in the electronic character of BA by complexation, as well as steric repulsion between BA and water. The ps time-resolved fluorescence measurements have shown that the TICT rate has no appreciable dependence on excitation energy or solvent isotopic substitution. This ob … More servation confirms that the TICT reaction proceeds via "sequential" mechanism ; the initially prepared level is predominately coupled to intermediate levels with high vibrational excitation of torsional motion, which further relax to the final levels in the charge-separated state. This result demonstrates the importance of the torsional motion in the dynamics of TICT reactions.
2. The water-solvated clusters of 9-acridone (AD) have been studied to explore the microscopic solvation effect on inter-system crossing (ISC) in AD.The fluorescence quantum yield is greatly enhanced with increasing order of solvation. Especially, drastic change with>200-fold increase caused by addition of only one water to the monomer indicates the crossover of the reaction mechanism form the direct ISC to the second-order ISC.Structural characterization by JR-UV double resonance spectroscopy combined with ab initio MO calculation has shown that water is hydrogen-bonded to C=O of AD in the 1 : 1 cluster. These results validates the site-selective microsolvation effect on ISC. Less

Report

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

    (27 results)

All Other

All Publications (27 results)

  • [Publications] H.Kohguchi,et al.: "Laser-induced-fluorescence spectra and observation of the quantum beats in the A ^2II_i-X^2II_i transition of the HCCS radical" Chemical Physics Letters. 254. 397-402 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Y.Ohshima,et al.: "Rotational spectroscopy of jet-cooled molecular ions and ion complexes" Chemical Physics Letters. 256. 635-640 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Y.Ohshima,et al.: "Rotational spectroscopy of the Ar-HCO^+ ionic complex" The Journal of Chemical Physics. 106. 2977-2979 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] H.Kohguchi,et al.: "Laser-induced-fluorescence spectroscopy of the C^2Σ^+-X^2II_<1/2> band system of the CCN radical in a supersonic jet" The Journal of Chemical Physics. 106. 5429-5438 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] K.Tanaka,et al.: "Pulsed discharge nozzle Fourier transform microwave spectroscopy of the propargyl radical(H_2CCCH)" The Journal of Chemical Physics. 107. 2728-2733 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] M.Matumura,et al.: "Fourier-transform microwave spectroscopy of the argon-diacetylene van der Waals complex" Journal of Molecular Spectroscopy. 185. 178-184 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] H.Hoshina,et al.: "Laser-induced fluorescence spectroscopy of the C_4H and C_4D radicals in a supersonic jet" The Journal of Chemical Physics. 108. 3465-3478 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] A Mizoguchi,et al.: "Rotational spectrum of a salt-containing van der Waals complex: Ar-NaCl" The Journal of Chemical Physics. 109. 10539-10542 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] K.Tanaka,et al.: "Determination of the proton tunneling splitting of tropolone in the ground state by microwave spectroscopy" The Journal of Chemical Physics. 110. 1969-1978 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] H.Kohguchi, et al.: "Laser-induced-fluorescence spactra and observation of the quantum beats in the A ^2P_i-X^2P_i transition of the HCCS radical" Chemical Physics Letters. 254. 397-402 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Y.Ohshima, et al.: "Rotational spectroscopy of jet-cooled molecular ions and ion complexes" Chemical Physics Letters. 256. 635-640 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] Y.Ohshima, et al.: "Rotational spectroscopy of the Ar-HCO^+ ionic complex" The Journal of Chemical Physics. 106. 2977-2979 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] H.Kohguchi, et al.: "Laser-induced-fluorescence spectroscopy of the C^2SIGMA^+-X^2P_<1/2> band system of the CCN radical in a supersonic jet" The Journal of Chemical Physics. 106. 5429-5438 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] K.Tanaka, et al.: "Pulsed discharge nozzle Fourier transform microwave spectroscopy of the propargyl radical (H_2CCCH)" The Journal of Chemical Physics. 107. 2728-2733 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] M.Matumura, et al.: "Fourier-transform microwave spectroscopy of the argon-diacetylene van der Waals complex" Journal of Molecular Spectroscopy. 185. 178-184 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] H.Hoshina, et al.: "Laser-induced fluorescence spectroscopy of the C_4H and C_4D radicals in a supersonic jet" The Journal of Chemical Physics. 108. 3465-3478 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] A.Mizoguchi, et al.: "Rotational spectrum of a salt-containing van der Waals complex : Ar-NaCl" The Journal of Chemical Physics. 109. 10539-10542 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] K.Tanaka, et al.: "Determination of the proton tunneling splitting of tropolone in the ground state by microwave spectroscopy" The Journal of Chemical Physics. 110. 1969-1978 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1997 Final Research Report Summary
  • [Publications] H.Kohguchi, et al.: "Laser-induced-fluorescence spectroscopy of the C^2Σ^+-Χ^2Π_<1/2> band system of the CCN radical in a supersonic jet" The Journal of Chemical Physics. 106. 5429-5438 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] K.Tanaka, et al.: "Pulsed discharge nozzle Fourier transform microwave spectroscopy of the propargyl radical (H_2CCCH)" The Journal of Chemical Physics. 107. 2728-2733 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] M.Matumura, et al.: "Fourier-transform microwave spectroscopy of the argon-diacetylene van der Waals complex" Journal of Molecular Spectroscopy. 185. 178-184 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] H.Hoshina, et al.: "Laser-induced fluorescence spectroscopy of the C_4H and C_4D radicals in a supersonic jet" The Journal of Chemical Physics. 108. 3465-3478 (1998)

    • Related Report
      1997 Annual Research Report
  • [Publications] H.Kohguchi,et al.: "Laser-induced-fluorescence spectra and olaservation of quantum beats in the A^1π^1-X^2π transition of the HCCS radical" Chemical Physics Letters. 254. 397-402 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] Y.Ohshima,et al.: "Rotational spectroscopy of jet-cooled molecular ions and ion complexes" Chenical Physics Letters. 256. 635-640 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] H.Ishikawa,et al.: "Stimulated emission pumping spectroscopy of HCP near the isomerization barrier : Evig 【less than or equal】 25315cm^< " The Journal of Chemical Physics. 105. 7383-7401 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] Y.Ohshima,et al.: "Rotational spectrunm of the Ar-HCO^+ ionic complex" The Journal of Chemical Physics. 106. 2977-2979 (1997)

    • Related Report
      1996 Annual Research Report
  • [Publications] H.Kohguchi,et al.: "Laser-irduced-fluorescence spectroscopy of the C^2E^+-X^2π4_2 bard system of the CCN raoicol in a supersoric jct" The Journal of Chemical Physics22GD05:(in press). (1997)

    • Related Report
      1996 Annual Research Report

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Published: 1996-04-01   Modified: 2016-04-21  

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