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Statistical Spectroscopy of Quantum Chaos State in Vibrationally Highly Excited polyatomic Molecules

Research Project

Project/Area Number 02044038
Research Category

Grant-in-Aid for international Scientific Research

Allocation TypeSingle-year Grants
SectionJoint Research
Research InstitutionThe University of Tokyo

Principal Investigator

TSUCHIYA Soji  College of Arts and Sciences, the University of Tokyo, 教養学部, 教授 (40012322)

Co-Investigator(Kenkyū-buntansha) LUNDBERG J. K.  Department of Chemistry, Massachusetts Institute of Technology, 化学科, 助手
JOST R.  Lab. Spectrometric Phys., University of Joseph-fourier Grenoble I, グルノーブル, 主任研究員
PIQUE J. P.  Lab. Spectrometric Phys., University of Joseph-Fourier Grenoble I, グルノーブル, 主任研究員
LOMBARDI M.  Lab. Spectrometric Phys., University of Joseph-Fourier Grenoble I, グルノーブル, 主任研究員
JOUVET C.  Lab. Molecular Photophys., University of Paris-Sud, 光分子物理研究室, 主任研究員
SOEP B.  Lab. Molecular Photophys., University of Paris-Sud, 光分子物理研究室, 主任研究員
HELLER E. J.  Department of Chemistry, University of Washington, 化学科, 教授
FIELD R. W.  Department of Chemistry, Massachusetts Institute of Technology, 化学科, 教授
OHSHIMA Yasuhiro  College of Arts and Sciences, the University of Tokyo, 教養学部, 助手 (60213708)
KANAMORI Hideto  College of Arts and Sciences, the University of Tokyo, 教養学部, 助手 (00204545)
YAMANOUCHI Kaoru  College of Arts and Sciences, the University of Tokyo, 教養学部, 助教授 (40182597)
ENDO Yasuki  College of Arts and Sciences, the University of Tokyo, 教養学部, 助教授 (40106159)
Project Period (FY) 1990 – 1991
Project Status Completed (Fiscal Year 1991)
Budget Amount *help
¥5,400,000 (Direct Cost: ¥5,400,000)
Fiscal Year 1991: ¥2,500,000 (Direct Cost: ¥2,500,000)
Fiscal Year 1990: ¥2,900,000 (Direct Cost: ¥2,900,000)
KeywordsChaos / Molecular Vibration / Laser spectroscopy / Unimolecular Reaction / van der Waals complex / カオス / 振動高励起分子
Research Abstract

This project aims at cooperative experimental and theoretical studies on intramolecular vibrational dynamics of highly excited polyatomic molecules which have been carried out in four laboratories of Tokyo, Cambridge, Grenoble and Paris.
1. Vibrational dynamics of highly excited acetylene
(1) MIT group proposed a chaotic vibrational dynamics by means of a statistical analysis of level energies of vibrationally highly excited acetylene.
(2) Grenoble group claimed an incomplete chaotic dynamics of excited acetylene based on the Fourier analysis of the spectral data obtained by MIT group.
(3) Tokyo group observed a dispersed fluorescence spectrum of acetylene in a single rovibronic level to obtain a global feature of the vibrational level structure. They could analyze it in terms of an anharmonic expansion function assuming five normal modes in an energy region up to around 14, 000 cm^<-1>. Beyond this energy, two CH bending, modes (trans and cis) couple each other, so that a local chaotic dy … More namics is realized within these modes. Couplings to other modes occur in another stage approaching a final full chaotic dynamics.
(4) Following the above proposal, MIT group confirmed an anharmonic coupling scheme between two CH stretching modes based on the high-resolution SEP spectrum of acetylene.
2. Unimolecular dissociation reaction of NO_2
(1) Tokyo group succeeded to take a state-selected photofragment (O or NO) excitation spectrum of NO_2. The observed spectrum showed a line structure which indicated the dissociation reaction via highly excited vibrational states of N0_2.
(2) The vibrational level structure of excited N0_2 was discussed by Grenoble group, who predicted a chaotic level structure even in the region below the dissociation threshold.
3. Structure and dynamics of electronically excited van der Waals complexes
(1) Tokyo group predicted the structure of HgAr_2 complex by means of LIF spectroscopy and optical-optical double resonance method.
(2) Orsay group discussed the structure of HgAr_2 based on a semi-empirical calculation of the potential surface as well as resonantly enhanced multiple photon ionization method. Less

Report

(3 results)
  • 1991 Annual Research Report   Final Research Report Summary
  • 1990 Annual Research Report
  • Research Products

    (19 results)

All Other

All Publications (19 results)

  • [Publications] N.Ochi et al.: "Rovibronic level structure of electronically excited acetylene(A ^1A_u) in a supersonic jet" Chem.Phys.152. 319-336 (1991)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] P.Dupre et al.: "Anomalous behavior of the anticrossing density as a function of excitation energy in the C_2H_2 molecule" Chem.Phys.152. 293-318 (1991)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] J.Miyawaki et al.: "Photofragment excitation spectrum of NO_2 observed through O( ^3P_J) detection" Chem.Phys.Lett.180. 287-292 (1991)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] K.Yamanouchi et al.: "Vibrationally highly excited acetylene as studied by dispersed fluorescence and stimulated emission pumping spectroscopy:Vibrational assignment of feature states" J.Chem.Phys.95. 6330-6342 (1991)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] M.Momona et al.: "High resolution study of the perturbation in the CO triplet band" J.Mol.Spectrosc.

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] D.J.Jonas et al.: "Intramolecular vibrational relaxation and forbidden transitions in the SEP spectrum of acetylene" J.Chem.Phys.

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] N. Ochi et al.: "Rovibronic level structure of electronically excited acetylene (A ^1A_u) in a supersonic jet" Chem. Phys.152. 319-336 (1991)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] P. Dupre et al.: "Anomalous behavior of the anticrossing density as a function of excitation energy in the C_2H_2 molecule" Chem. Phys.152. 293-318 (1991)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] J. Miyawaki et al.: "Photofragment excitation spectrum of NO_2 observed through O ( ^3P) detection" Chem. Phys. Lett.180. 287-292 (1991)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] K. Yamanouchi et al.: "Vibrationally highly excited acetylene as studied by dispersed fluorescence and stimulated emission pumping spectroscopy : Vibrational assignment of feature states" J. Chem. Phys.95. 6330-6342 (1991)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] M. Momona et al.: "High resolution study of the perturbation in the CO triplet band" J. Mol. spectrosc.(1992)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] D. J. Jonas et al.: "Intramolecular vibrational relaxation and forbidden transitions in the SEP spectrum of acetylene" J. Chem. Phys.

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1991 Final Research Report Summary
  • [Publications] K.Yamanouchi et al.: "Vibrationally highly excited acethlene as studied by dispersed fluorescence and stimulated emission pumping spectroscopy:Vibrational assignment of the feature states" J.Chem.Phys.95. 6330-6342 (1991)

    • Related Report
      1991 Annual Research Report
  • [Publications] M.Momona et al.: "High resolution study of the perturbation in the CO triplet band" J.Mol.Spectrosc.

    • Related Report
      1991 Annual Research Report
  • [Publications] D.J.Jonas et al.: "Intramolecular vibrational relaxation and forbidden transitions in the SEP spectrum of acetylene" J.Chem.Phys.

    • Related Report
      1991 Annual Research Report
  • [Publications] 土屋 荘次: "励起分子の量子ビ-ト分光" 分光研究. 41. 3-20 (1992)

    • Related Report
      1991 Annual Research Report
  • [Publications] N.Ochi et al.: "Rovibronic level structure of electronically excited acetylene (A^lA_u) in a supersonic jet" Chem.Phys.). 02%33 (1991)

    • Related Report
      1990 Annual Research Report
  • [Publications] J.Miyawaki et al.: "Photofragment excitation spectrum of NO_2 observed through O(^3P_J) detection" Chem.Phys.Lett.). 02%33 (1991)

    • Related Report
      1990 Annual Research Report
  • [Publications] P.Dupre et al.: "Anomalous behavior of the anticrossing density as a function of excitation energy in the C_2H_2 molecule" Chem.Phys.). 02%33 (1991)

    • Related Report
      1990 Annual Research Report

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Published: 1990-04-01   Modified: 2016-04-21  

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