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Clarification of the uniqueness of supercritical water from the view point of energy transfer dynamics

Research Project

Project/Area Number 16350010
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

KIMURA Yoshifumi  Kyoto University, International Innovation Center, Associate Professor, 国際融合創造センター, 助教授 (60221925)

Project Period (FY) 2004 – 2006
Project Status Completed (Fiscal Year 2006)
Budget Amount *help
¥13,600,000 (Direct Cost: ¥13,600,000)
Fiscal Year 2006: ¥2,000,000 (Direct Cost: ¥2,000,000)
Fiscal Year 2005: ¥1,800,000 (Direct Cost: ¥1,800,000)
Fiscal Year 2004: ¥9,800,000 (Direct Cost: ¥9,800,000)
Keywordssupercritical water / supercritical alcohols / optical Kerr gate / time-resolved fluorescence / vibrational relaxation / perylene / Raman spectroscopy / nitroaniline / 超臨界水 / 超臨界アルコール / 過渡回折格子法 / エネルギー移動 / 光カーゲート法 / 超臨界流体 / イオン液体 / アクセプター数
Research Abstract

We have developed an optical Kerr gate system for the time-resolved fluorescence detection under high-temperature and high-pressure fluids such as supercritical water (SCW) and supercritical methanol (SCMe). Using a third-harmonic output from a Ti : Sapphire laser as pump pulse and a fundamental output as a gate pulse, we attained the time-resolution of 1.2 ps by using a glass with high refractive index as a Kerr medium. We applied the system for the measurement of the fluorescence dynamics of perylene in SCMe, and found that the initial variation of the spectrum shape after the photo-excitation. The change was interpreted as the energy dissipation process by comparing the excess energy dependence of the fluorescence lineshape in vapor. The vibrational energy dissipation (VER) rate thus determined varied little by changing the solvent density from the critical density to twice of it, while the temperature effect on VER rate was large. The mechanism of VER was also investigated by other non-linear laser spectroscopy.
We have also measured Raman spectra of p-nitroaniline in SCW and SCMe. Based on Raman spectra of chemical compounds with similar molecular structures measured in various solvents, we found that the vibrational frequency of the NO_2 stretching mode was strongly affected by the bulk property of solvent such as the dielectric constant, while the vibrational frequency of the NH_2 stretching mode was strongly affected by the hydrogen-bonding from the solvent molecule. The similarity of the density dependence of the VER rate of perylene to the vibrational spectral shift of NH_2 mode of p-ntroaniline may suggests the VER through the hydrogen-bonding is effective in SCMe.
In the future, we are planning to measure the VER rate in SCW which could not be tried within the period of this program, and investigate the mechanism of VER more intimately with the vibrational spectroscopy.

Report

(4 results)
  • 2006 Annual Research Report   Final Research Report Summary
  • 2005 Annual Research Report
  • 2004 Annual Research Report
  • Research Products

    (32 results)

All 2007 2006 2005 2004 Other

All Journal Article (32 results)

  • [Journal Article] Application of the transient grating method to the investigation of the photo-thermalization process of malachite green in room temperature ionic liquids2007

    • Author(s)
      M.Fukuda, O.Kajimoto, M.Terazima, Y.Kimura
    • Journal Title

      Journal of Molecular Liquids 134

      Pages: 49-49

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Photo-excitation dynamics of malachite green in ionic liquids studied by the transient grating method2007

    • Author(s)
      M.Fukuda, O.Kajimoto, M.Terazima, Y.Kimura
    • Journal Title

      Ultrafast Phenomena XV (in press)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Annual Research Report 2006 Final Research Report Summary
  • [Journal Article] Application of the transient grating method to the investigation of the photo-thermalization process of malachite green in room temperature ionic liquids2007

    • Author(s)
      M.Fukuda, O.Kajimoto, M.Terazima, Y.Kimura
    • Journal Title

      Journal of Molecular Liquids 134(1-3)

      Pages: 49-49

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Application of the transient grating method to the investigation of the photo-thermalization process of malachite green in room temperature ionic liquids2007

    • Author(s)
      M.Fukuda, O.Kajimoto, M.Terazima, Y.Kimura
    • Journal Title

      Journal of Molcular Liquids 134

      Pages: 49-49

    • Related Report
      2006 Annual Research Report
  • [Journal Article] 超臨界流体中における非線形レーザー分光2006

    • Author(s)
      木村佳文, 網田富士嗣, 藤澤知績
    • Journal Title

      高圧力の科学と技術 16

      Pages: 87-87

    • NAID

      10017568598

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Raman spectroscopic study on solvation of Diphenylcyclopropenone and Phenol Blue in room temperature ionic liquids2006

    • Author(s)
      T.Fujisawa, M.Fukuda, M.Terazima, Y.Kimura
    • Journal Title

      Journal of Physical Chemistry A 110

      Pages: 6114-6114

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Resonance Raman study of the solvation of p-nitroaniline in supercritical water2006

    • Author(s)
      T.Fujisawa, M.Terazima, Y.Kimura, M.Maroncelli
    • Journal Title

      Chemical Physics Letters 430

      Pages: 303-303

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Annual Research Report 2006 Final Research Report Summary
  • [Journal Article] Study on the vibrational energy relaxation of p-nitroaniline, N,N-dimethyl-p-nitroaniline and azulene by the transient grating method2006

    • Author(s)
      Y, Kimura, M.Fukuda, O.Kajimoto, M.Terazima
    • Journal Title

      The Journal of Chemical Physics 125

      Pages: 194516-194516

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Excitation wavelength dependence of the Raman Stokes shift of N,N-dimethyl-p-nitroaniline2006

    • Author(s)
      T.Fujisawa, M.Terazima, Y.Kimura
    • Journal Title

      The Journal of Chemical Physics 124

      Pages: 184503-184503

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Raman spectroscopic study on solvation of diphenylcyclopropenone and phenol blue in room temperature ionic liquids2006

    • Author(s)
      T.Fujisawa, M.Fukuda, M.Terazima, Y.Kimura
    • Journal Title

      Journal of Physical Chemistry A 110(18)

      Pages: 6164-6172

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Excitation wavelength dependence of the Raman Stokes shift of N,N-dimethyl-p-nitroaniline2006

    • Author(s)
      T.Fujisawa, M.Terazima, Y.Kimura
    • Journal Title

      The Journal of Chemical Physics 124(18)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Resonance Raman study of the solvation of p-nitroaniline in supercritical water2006

    • Author(s)
      T.Fujisawa, M.Terazima, Y.Kimura, M.Maroncelli
    • Journal Title

      Chemical Physics Letter 430

      Pages: 303-308

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Study on the vibrational energy relaxation of p-nitroaniline, N,N-dimethyl-p-nitroaniline and azulene by the transient grating method2006

    • Author(s)
      Y.Kimura, M.Fukuda, O.Kajimoto, M.Terazima
    • Journal Title

      The Journal of Chemical Physics. 125

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Non-linear laser spectroscopy in supercritical fluids2006

    • Author(s)
      Y.Kimura, F.Amita, T.Fujisawa
    • Journal Title

      Review of High Pressure Science and Technology 16(2)

      Pages: 87-94

    • NAID

      10017568598

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Study on the vibrational energy relaxation of p-nitroaniline, N,N-dimethyl-p-nitroaniline and azulene by the transient grating method2006

    • Author(s)
      Y.Kimura, M.Fukuda, O.Kajimoto, M.Terazima
    • Journal Title

      Journal of Chemical Physics 125

      Pages: 194516-194516

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Excitation wavelength dependence of the Raman Stokes shift of N,N-dimethyl-p-nitroaniline2006

    • Author(s)
      T.Fujisawa, M.Terazima, Y.Kimura
    • Journal Title

      The Journal of Chemical Physics (in press)

    • Related Report
      2005 Annual Research Report
  • [Journal Article] 超臨界流動体中における非線形レーザー分光2006

    • Author(s)
      木村佳文, 網田富士嗣, 藤澤知績
    • Journal Title

      高圧力の科学と技術 (in press)

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Raman spectroscopic study on solvation of Diphenylcyclopropenone and Phenol Blue in room temperature ionic liquids2006

    • Author(s)
      T.Fujisawa, M.Fukuda, M.Terazima, Y.Kimura
    • Journal Title

      Journal of Physical Chemistry A (in press)

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Acceptor Number of Room Temperature Ionic Liquid Determined by the Raman Spectrum of Diphenylcyclopropenone2005

    • Author(s)
      Y.Kimura, M.Fukuda, T.Fujisawa, M.Terazima
    • Journal Title

      Chemistry Letters 34(3)

      Pages: 338-338

    • NAID

      10014464362

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Development and Application of the Multipurpose Optical Flow Cell under Supercritical Condition of Water2005

    • Author(s)
      T.Fujisawa, E.Maru, F.Amita, M.Harada, T.Uruga, Y.Kimura
    • Journal Title

      Water, Steam, and Aqueous Solutions for Electric Power 14

      Pages: 445-445

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Vibrational energy relaxation of azulene studied by the transient grating method. I. Supercritical fluids2005

    • Author(s)
      Y.Kimura, Y.Yamamoto, H.Fujiwara, M.Terazima
    • Journal Title

      The Journal of Chemical Physics 123

      Pages: 54512-54512

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Vibrational energy relaxation of azulene studied by the transient grating method. II. Liquid Solvents2005

    • Author(s)
      Y.Kimura, Y.Yamamoto, M.Terazima
    • Journal Title

      The Journal of Chemical Physics 123

      Pages: 54513-54513

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Acceptor number of room temperature ionic liquid determined by the Raman spectrum of diphenylcyclopropenone2005

    • Author(s)
      Y.Kimura, M.Fukuda, T.Fujisawa, M.Terazima
    • Journal Title

      Chemistry Letters 34(3)

      Pages: 338-339

    • NAID

      10014464362

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Development and Application of the Multipurpose Optical Flow Cell under Supercritical Condition of Water2005

    • Author(s)
      T.Fujisawa, E.Maru, F.Amita, M.Harada, T.Uruga, Y.Kimura
    • Journal Title

      Water, Steam, and Aqueous Solutions for Electric Power(edited by M.Nakahara, N.Matubayashi, M.Ueno, K.Yasuoka, K.Watanabe)

      Pages: 445-450

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Vibrational energy relaxation of azulene studied by the transient grating method. I. Supercritical fluids2005

    • Author(s)
      Y.Kimura, Y.Yamamoto, H.Fujiwara, M.Terazima
    • Journal Title

      The Journal of Chemical Physics 123(5)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Vibrational energy relaxation of azulene studied by the transient grating method. II. Liquid Solvents2005

    • Author(s)
      Y.Kimura, Y.Yamamoto, M.Terazima
    • Journal Title

      The Journal of Chemical Physics 123(5)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Vibrational energy relaxation of azulene studied by the transient grating method. I. Supercritical Fluids2005

    • Author(s)
      Y.Kimura, Y.Yamamoto, H.Fujiwara, M.Terazima
    • Journal Title

      The Journal of Chemical Physics 123(5)

      Pages: 54512-54512

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Acceptor Number of Room Temperature Ionic Liquid Determined by the Raman Spectrum of Diphenylcyclopropenone2005

    • Author(s)
      Y.Kimura, M.Fukuda, T.Fujisawa, M.Terazima
    • Journal Title

      Chemistry Letters 34・(3)

      Pages: 338-338

    • NAID

      10014464362

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Photo-thermalization dynamics of azulene in supercritical fluids studied by the transient grating method2004

    • Author(s)
      Y.Kimura, Y.Yamamoto, M.Terazima
    • Journal Title

      Ultrafast Phenomena XIV

      Pages: 398-398

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Photo-thermalization dynamics of azulene in supercritical fluids studied by the transient grating method2004

    • Author(s)
      Y.Kimura, Y.Yamamoto, M.Terazima
    • Journal Title

      Ultrafast Phenomena XIV(edited by T. Kobayashi, T.Okada, T.Kobayashi, K.A. Nelson, S.DeSilverstri)(Springer)

      Pages: 398-400

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Photo-excitation dynamics of malachite green in ionic liquids studied by the transient grating method

    • Author(s)
      M.Fukuda, O.Kajimoto, M.Terazima, Y.Kimura
    • Journal Title

      Ultrafast Phenomena XV (in press)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Photo-thermalization dynamics of azulene in supercritical fluids studied by the transient grating method

    • Author(s)
      Y.Kimura, Y.Yamamoto, M.Terazima
    • Journal Title

      Ultrafast Phenomena XIV, 2005 (in press)

    • Related Report
      2004 Annual Research Report

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Published: 2004-04-01   Modified: 2016-04-21  

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