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2002 Fiscal Year Final Research Report Summary

Basic measurements of partial orders in solution

Research Project

Project/Area Number 12440158
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

Principal Investigator

IWATA Koichi  The University of Tokyo, Graduate School of Science, Associate Professor, 大学院・理学系研究科, 助教授 (90232678)

Project Period (FY) 2000 – 2002
Keywordsmicelle / SDS / trans-stilbene / solution / carbon tetrachloride / diffusion-controlled reaction / femtosecond / time-resolved near-infrared spectroscopy
Research Abstract

Kinetics of bimolecular chemical reactions between trans-stilbene or biphenyl and carbon tetrachloride have been measured with femtosecond time-resolved spectroscopic methods. The observed kinetics are well explained by theories of diffusion-controlled reactions. This result suggests that the translational motion of molecules in solution is described well as diffusion motion after a few picosecond time interval.
Mechanism of a double proton transfer reaction induced by photoexcitation of the 2-aminopyridin / acetic acid complex has been examined. Experimental results from picosecond time-resolved spectroscopy show that this double proton transfer proceeds with a stepwise mechanism. It is crucial to keep the molecular complex between 2-aminopyridine and acetic acid for at least a few picoseconds for this reaction.
Temperature dependence of the trans-cis isomerization rate as well as the shape of the Raman bands of the first excited singlet (S_1) state of trans-stilbene have been measured in three different solvents, hexane, octane, and decane. The relation between the isomerization reaction rate and the solute-solvent interaction is discussed based on the experimental results. The dynamic polarization model, which postulates that the amplitude, duration, and frequency of the solute-solvent interaction determine both the reaction rate and the Raman band shape, explains the experimental results successfully.
Trans-stilbene solubilized in the hydrophobic core of the SDS micelle is ionized by photoexcitation. From the picosecond time-resolved CARS experiments, it has been suggested strongly that the generated cation radial reaches the outer hydrophilic interface between the micelle and the bulk water within 20 ps. It has been also suggested, however, that it takes 1 to 2 ps for the electron generated simultaneously with the cation radial to reach the bulk water.

  • Research Products

    (12 results)

All Other

All Publications (12 results)

  • [Publications] Koichi Iwata, Hiroaki Takahashi: "Photoinduced Cl transfer reaction between biphenyl and carbon tetrachloride studied by nanosecond time-resolved infrared spectroscopy and picosecond time-resolved fluorescence spectroscopy"Journal of Molecular Structure. 598. 97-102 (2001)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] Koichi Iwata, Satoshi Takeuchi, Tahei Tahara: "Photochemical bimolecular reaction between biphenyl and carbon tetrachloride : observed ultrafast kinetics and diffusion-controlled reaction model"Chemical Physics Letters. 347. 331-336 (2001)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] Hironori Ishikawa, Koichi Iwata, Hiro-o Hamaguchi: "Picosecond dynamics of stepwise double proton transfer reaction in the excited state of the 2-aminopyridine/acetic acid system"Journal of Physical Chemistry A. 106. 2305-2312 (2002)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] Koichi Iwata, Ryosuke Ozawa, Hiro-o Hamaguchi: "Analysis of the solvent-and temperature-dependent Raman spectral changes of S_1 trans-stilbene and the mechanism of the trans to cis isomerization : dynamic polarization model of vibrational dephasing and the C=C double-bond rotation"Journal of Physical Chemistry A. 106. 3614-3620 (2002)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] Koichi Iwata: "Effects of pump and probe light field on picosecond time-resolved resonance Raman spectra of S_1 trans-stilbene. Disagreement between Stokes-and anti-Stokes scattering frequencies"Bulletin of the Chemical Society of Japan. 75. 1075-1082 (2002)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] Hiro-o Hamaguchi, Koichi Iwata: "Physical Chemistry of S_1 trans-Stilbene in Solution as Studied by Time-resolved Raman Spectroscopy"Bulletin of the Chemical Society of Japan. 75. 883-897 (2002)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] IWATA, Koichi, TAKAHASHl, Hiroaki: "Photoinduced Cl transfer reaction between biphenyl and carbon tetrachloride studied by nanosecond time-resolved infrared spectroscopy and picosecond time-resolved fluorescence spectroscopy"Journal of Molecular Structure. 598. 97-102 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] IWATA, Koichi, TAKEUCHI, Satoshi, TAHARA, Tahei: "Photochemical bimolecular reaction between biphenyl and carbon tetrachloride : observed ultrafast kinetics and diffusion-controlled reaction model"Chemical Physics Letters. 347. 331-336 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] ISHKAWA, Hironori, IWATA, Koichi, HAMAGUCHI Hiro-o: "Picosecond dynamics of stepwise double proton transfer reaction in the excited state of the 2-aminopyridine/acetic acid system"Journal of Physical Chemistry A. 106. 2305-2312 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] IWATA, Koichi, OZAWA, Ryosuke, HAMAGUCHI Hiro-o: "Analysis of the solvent- and temperature-dependent Raman spectral changes of S_1 trans-stilbene and the mechanism of the trans to cis isomerization : dynamic polarization model of vibrational dephasing and the C=C double-bond rotation"Journal of Physical Chemistry A. 106. 3614-3620 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] IWATA, Koichi: "Effects of pump and probe light field on picosecond time-resolved resonance Raman spectra of S_1 trans-stilbene. Disagreement between Stokes- and anti-Stokes scattering frequencies"Bulletin of the Chemical Society of Japan. 75. 1075-1082 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] HAMAGUCHI Hiro-o, IWATA, Koichi: "Physical Chemistry of S_1 trans-Stilbene in Solution as Studied by Time-resolved Raman Spectroscopy"Bulletin of the Chemical Society of Japan. 75. 883-897 (2002)

    • Description
      「研究成果報告書概要(欧文)」より

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Published: 2004-04-14  

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