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MEASUREMENTS OF STATE-RESOLVED DIFFERENTIAL CROSS SECTIONS VIA HIGH-RESOLUTION POLARIZED DOPPLER SPECTROSCOPY

Research Project

Project/Area Number 09640600
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeSingle-year Grants
Section一般
Research Field Physical chemistry
Research InstitutionKYOTO UNIVERSITY

Principal Investigator

FUJIMURA Yo  Kyoto University, Chemistry, Research Associate, 大学院・理学研究科, 助手 (00222266)

Co-Investigator(Kenkyū-buntansha) KAJIMOTO Okitsugu  Kyoto University, Chemistry, Professor, 大学院・理学研究科, 教授 (30029483)
Project Period (FY) 1997 – 1998
Project Status Completed (Fiscal Year 1998)
Budget Amount *help
¥3,300,000 (Direct Cost: ¥3,300,000)
Fiscal Year 1998: ¥500,000 (Direct Cost: ¥500,000)
Fiscal Year 1997: ¥2,800,000 (Direct Cost: ¥2,800,000)
KeywordsOxygen / Nitrous Oxide / Hydrogen / Hydrocarbon / Water / Reaction Dynamics / Doppler Spectroscopy / Differential Cross Sections
Research Abstract

Chemical reaction dynamics of elementary gas phase reactions have been studied via Dopplerresolved polarization spectroscopy. By using this technique, differential cross sections can be measured state-resolved manner. Furthermore, this method enables us to measure the polarization of the rotational angular momentum of reaction products.
Collision-free diatomic product molecules were probed with high-resolution dye laser excitation and its Doppler-broadened line profiles were analyzed to extract the information of vector properties such as differential cross sections and rotational angular momentum polarization, We investigated the reaction of O(^1D) atom with some several simple molecules. Following results are shown. 1) For H_2 reaction, differential cross sections and collision energy dependence of reaction probability strongly depend on ro-vibrational states of product OH molecules. Critical comparison with a quasi-classical trajectory calculation on a recent state-of-the-art ab init … More io potential energy surfaces. 2) For N_2O reaction, efficient energy randomization within all the degrees of freedom of reaction intermediates leads apparent statistical ro-vibrational state distribution of product NO molecules despite the absence of a deep potential well. Such a behavior is generally interpreted in terms of intermolecular vibrational-energy redistribution, with the emphasis of the light (hydrogen) atom effect. 3) For C_2H_4 and C_2H_6 reaction, the difference of the structural change of reactive intermediates after the insertion of 0 atom forming alcohol type intermediates is reflected in the difference of the polarization of rotational angular momentum of product OH molecules. 4) For H_2O reaction, the main reaction path is an insertion of O atom into HO bond of H_2O forming HOGH as an intermediate.
To obtain such findings becomes possible only by the use of the state-resolved polarized Doppler spectroscopy. In addition, some of the findings in this study give new understandings which are opposite to the previous ones based on insufficient state-resolved measurements. The study elucidating elementary bimolecular reactions in this manner is essential for the fundamental understanding of chemical reaction dynamics. Less

Report

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

    (17 results)

All Other

All Publications (17 results)

  • [Publications] Andrew J.Alexander: "O(^1D_2)+H_2→OH|v'<=4, N'>+H: The anatomy of a reaction" Faraday Discussions. 108. 375-386 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] Hiroshi Akagi: "Vibrational distribution of highly vibrationally excited NO(X^2II)generated from the reaction of O(^1D)with N_2O" Journal of the Chemical Society Faraday Transactions. 94. 1575-1581 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] Hiroshi Tsurumaki: "Stereodynamics of the reactions of O(^1D)with C_2H_4 and C_2H_6" Chemical Physics Letters. 301. 145-152 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] Hiroshi Tsurumaki: "Stereodynamics of the vibrational channel O(^1D)+H_2O→OH(v'=2)+OH" The Journal of Chemical Physics. 110 in press. (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] Hiroshi Akagi: "Nascent state distributions of NO(X_2II)generated from the reaction of S(^1D)with N_<>_<>O : Intermolecular vibrational-energy redistribution(IVR)in the reaction" The Journal of Chemical Physics. 110 in press. (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] Andrew J.Alexander: "O(^1D_2)+H_2*OH|v'<=4, N'>+H : The anatomy of a reaction" Faraday Discussions. 108. 375-386 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] Hiroshi Akagi: "Vibrational distribution of highly vibrationally excited NO(X^2PI) generated from thereaction of O(^1D) with N_2O" Journal of the Chemical Society Faraday Transactions. 94. 1575-1581 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] Hiroshi Tsurumaki: "Stereodynamics of the reactions of O(^1D) with C_2H_4 and C_2H_4 and C_2H_6" Chemical Physics Letters. 301. 145-152 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] Hiroshi Tsurumaki: "Stereodynamics of the vibrational channel O(^1D)+H_2O*OH(V'=2)+OH" The Journal of Chemical Physics. 110(in press). (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] Hiroshi Akagi: "Nascent state distributions of NO(X^2PI) generated from the reaction of S(^1D) with N_2O : Intermolecular vibrational-energy redistribution (IVR) in the reaction" The Journal of Chemical Physics. 110(in press). (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] Hiroshi Akagi: "Vibrational distribution of highly vibrationally excited NO(X^2II)generated from the reaction of O(^1D)with N_2O" Journal of The Chemical Society Faraday Transaction. 98・11. 1575-1581 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] Hiroshi Tsurumaki: "Stereodynamics of the reactions of O(^1D)with C_2H_4 and C_2H_6" Chemical Physics Letters. 301・1,2. 145-152 (1999)

    • Related Report
      1998 Annual Research Report
  • [Publications] Hiroshi Tsurumaki: "Stereodynamics of the vibrational channel O(^1D)+H_2O→OH(v'=2)+OH" The Journal of Chemical Physics. 110・16(in press). (1999)

    • Related Report
      1998 Annual Research Report
  • [Publications] Hiroshi Akagi: "Nascent state distributions of NO(X^2II)generated from the reaction of S(^1D)with N_2O:Intermolecular vibrational-energy redistribution(IVR)in the reaction intermediate" The Journal of Chemical Physics. 110・16(in press). (1999)

    • Related Report
      1998 Annual Research Report
  • [Publications] Andrew J.Alexander: "O(^1D_2)+H_2→OH|υ',N'〉+H:The anatomy of a reaction." Faraday Discussion. 108(in press). (1998)

    • Related Report
      1997 Annual Research Report
  • [Publications] Takeki Ishida: "Excited state dynamics of 9,9'-byanthryl clusters with H_2O and Ar" Chemical Physics Letters. 286(in press). (1998)

    • Related Report
      1997 Annual Research Report
  • [Publications] Hiroshi Akagi: "Vibrational distribution of highly vibrationally excited NO molecules produced from O(^1D_2)+H_2O→NO+NO reaction" Journal of the Chemical Society Faraday Transactions. 94(in press). (1998)

    • Related Report
      1997 Annual Research Report

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

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