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Investigation of molecular multiply excited states and their quantum dynamics

Research Project

Project/Area Number 17350006
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field Physical chemistry
Research InstitutionTokyo Institute of Technology

Principal Investigator

KOUCHI Noriyuki  Tokyo Institute of Technology, Chem. Department, Professor (50161873)

Co-Investigator(Kenkyū-buntansha) KITAJIMA Masashi  Tokyo Institute of Technology, Chem. Department, Associate Professor (20291065)
ODAGIRI Takeshi  Tokyo Institute of Technology, Chem. Department, Assistant Professor (80282820)
Project Period (FY) 2005 – 2007
Project Status Completed (Fiscal Year 2007)
Budget Amount *help
¥12,580,000 (Direct Cost: ¥11,800,000、Indirect Cost: ¥780,000)
Fiscal Year 2007: ¥3,380,000 (Direct Cost: ¥2,600,000、Indirect Cost: ¥780,000)
Fiscal Year 2006: ¥3,000,000 (Direct Cost: ¥3,000,000)
Fiscal Year 2005: ¥6,200,000 (Direct Cost: ¥6,200,000)
Keywordsone-electron mean field approximation / Born-Oppenheimer approximation / multiply excited molecules / coincidence measurements / production of a photon-pair / electron collision / synchrotron radiation / NO / NH_3 / N_2 / O_2 / 原子・分子物理 / 量子エレクトロニクス / プラズマ・核融合 / 放射線、X線、粒子線 / 量子ビーム
Research Abstract

Revealing the multiple excitation in a molecule and subsequent decay of the multiply excited states is a challenging subject in physical chemistry since the independent electron model and the Born-Oppenheimer approximation are less available than in the electronic states below the first ionization potential We established the electron energy-loss spectroscopy tagged with photons and (γ, 2γ) spectroscopy, both of which are powerful for observing the multiply excited molecules. In the present work, we have aimed at investigating multiply excited molecules and their quantum dynamics. The molecules of interest range from diatomic molecules to polyatomic molecules.
We have measured the electron energy-loss spectra of CH_4 tagged with the Lyman-α photons at 80 eV incident electron energy and 12 and 24° electron scattering angle in the range of energy loss 20-46 eV. The peaks originating from doubly excited states have been observed as well as those originating from singly excited states. Interestingly, the former peaks are more intense than the latter ones. Angle-differential cross sections for the double excitation have been measured for the first time as a function of scattering angle, which depend on the scattering angle in a different manner from those of the single-excitation. Almost the same results were obtained for NH_3.
We have measured the cross sections for the generation of a pair of photons by a single photon absorption of an N_2 and an O_2 molecule as a function of incident photon energy in the range 23-50 eV. Peaks originating from multiply excited states have been observed. Interestingly, some of them lie in the range beyond the double ionization threshold.
We have concluded from the present work that the multiply excited states generally exist in a wide range of molecules and their quantum dynamics is not amenable to what we know about the singly excited molecules.

Report

(4 results)
  • 2007 Annual Research Report   Final Research Report Summary
  • 2006 Annual Research Report
  • 2005 Annual Research Report
  • Research Products

    (47 results)

All 2007 2006 2005

All Journal Article (27 results) (of which Peer Reviewed: 10 results) Presentation (20 results)

  • [Journal Article] The electron-energy-loss spectra of methane tagged with Lyman-α photons in the range of doubly excited states2007

    • Author(s)
      T. Nakazato, T. Odagiri, H. Fukuzawa, H. Miyagi, L. Ishikawa, M. Kitajima, and N. Kouchi
    • Journal Title

      Journal of Physics B: Atomic, Molecular and Optical Physics 40

      Pages: 2459-2470

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Theoretical study on the angular correlation of two Lyman-α photons generated by single-photon absorption of a hydrogen molecule2007

    • Author(s)
      H. Miyagi, A. Ichimura, and N. Kouchi
    • Journal Title

      Journal of Physics B: Atomic, Molecular and Optical Physics 40

      Pages: 617-628

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] The electron-energy-loss spectra of methane tagged with Lyman-α photons in the range of doubly excited states2007

    • Author(s)
      T., Nakazato, T., Odagiri, H., Fukuzawa, H., Miyagi, L., Ishikawa, M., Kitajima, N., Kouchi
    • Journal Title

      Journal of Physics B : Atomic, Molecular and Optical Physics 40(12)

      Pages: 2459-2470

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Journal Article] Theoretical study on the angular correlation of two Lyman-α photons generated by single-photon absorption of a hydrogen molecule2007

    • Author(s)
      H., Miyagi, A., Ichimura, N., Kouchi
    • Journal Title

      Journal of Physics B : Atomic, Molecular and Optical Physics 40(3)

      Pages: 617-628

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Journal Article] The electron-energy-loss spectra of methane tagged with Lyman-α photons in the range of doubly excited states2007

    • Author(s)
      T. Nakazato, T. Odagiri, H. Fukuzawa, H. Miyagi, L. Ishikawa, M. Kitajima, and N. Kouchi
    • Journal Title

      Journal of Physics B:Atomic, Molecular and Optical Physics 40

      Pages: 2459-2470

    • Related Report
      2007 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Theoretical study on the angular correlation of two Lyman-α photons generated by single-photon absorption of a hydrogen molecule2007

    • Author(s)
      H. Miyagi, A. Ichimura, and N. Kouchi
    • Journal Title

      Journal of Physics B:Atomic, Molecular and Optical Physics 40

      Pages: 617-628

    • Related Report
      2007 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Theoretical study on the angular correlation of two Lyman-a photons generated by single-photon absorption of a hydrogen molecule2007

    • Author(s)
      H.Miyagi, A.Ichimura, N.Kouchi
    • Journal Title

      Journal of Physics B : Atomic, Molecular and Optical Physics 40・3

      Pages: 617-628

    • Related Report
      2006 Annual Research Report
  • [Journal Article] 水素分子の2電子励起共鳴-未だに解けない基本の問題-2006

    • Author(s)
      小田切 丈、河内宣之
    • Journal Title

      日本物理学会誌 61

      Pages: 671-675

    • NAID

      110004793326

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Multiply excited states of molecular nitrogen in the vacuum ultraviolet range asstudied by(γ,2γ)method2006

    • Author(s)
      M. Murata, T. Odagiri and N. Kouchi
    • Journal Title

      Journal of Physics B: Atomic, Molecular and Optical Physics 39

      Pages: 1285-1297

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] (γ,2γ)studies on multiply excited states of H_2 and N_2 in the vacuum ultraviolet range2006

    • Author(s)
      T. Odagiri
    • Journal Title

      Ionization, Correlation, and Polarization in Atomic Collisions, AIP Conference Proceedings 811

      Pages: 156-160

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Doubly excited resonances in molecular hydrogen, - An outstanding problem of the simplest molecule-2006

    • Author(s)
      Takeshi, Odagiri, Noriyuki, Kouchi
    • Journal Title

      Butsuri 61(9)

      Pages: 671-675

    • NAID

      110004793326

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Journal Article] Multiply excited states of molecular nitrogen in the vacuum ultraviolet range as studied by (γ, 2γ) method2006

    • Author(s)
      M., Murata, T., Odagiri, N., Kouchi
    • Journal Title

      Journal of Physics B : Atomic, Molecular and Optical Physics 39(6)

      Pages: 1285-1297

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Journal Article] (γ, 2γ) studies on multiply excited states of H_2 and N_2 in the vacuum ultraviolet range2006

    • Author(s)
      T., Odagiri
    • Journal Title

      Ionization, Correlation, and Polarization in Atomic Collisions, AIP Conference Proceedings 811

      Pages: 156-160

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Journal Article] Multiply excited states of molecular nitrogen in the vacuum ultraviolet range as studied by (γ,2γ) method2006

    • Author(s)
      M.Murata, T.Odagiri, N.Kouchi
    • Journal Title

      Journal of Physics B : Atomic, Molecular and Optical Physics 39・6

      Pages: 1285-1297

    • Related Report
      2006 Annual Research Report
  • [Journal Article] (γ,2γ) studies on multiply excited states of H2 and N2 in the vacuum ultraviolet range2006

    • Author(s)
      T.Odagiri
    • Journal Title

      Ionization,Correlation,and Polarization in Atomic Collisions, AIP Conference Proceedings 811

      Pages: 156-160

    • Related Report
      2006 Annual Research Report
  • [Journal Article] 水素分子の2電子励起共鳴2006

    • Author(s)
      小田切 丈, 河内宣之
    • Journal Title

      日本物理学会誌 61・9

      Pages: 671-675

    • Related Report
      2006 Annual Research Report
  • [Journal Article] (γ,2γ) studies on multiply excited states of H_2 and N_2 in the vacuum ultraviolet range2006

    • Author(s)
      Takeshi Odagiri
    • Journal Title

      AIP CONFERENCE PROCEEDINGS 881

      Pages: 156-160

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Multiply excited states of molecular nitrogen in the vacuum ultraviolet rang as studied by (γ,2γ) method2006

    • Author(s)
      Makoto Murata, Takeshi Odagiri, Noriyuki Kouchi
    • Journal Title

      J.Phys B : At.Mol.Opt.Phys. 39

      Pages: 1285-1297

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Doubly excited states of methane produced by photon and electron interactions2005

    • Author(s)
      H. Fukuzawa, T. Odagiri, T. Nakazato, M. Murata, H. Miyagi and N. Kouchi
    • Journal Title

      Journal of Physics B: Atomic, Molecular and Optical Physics 38

      Pages: 565-578

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Measurements of the fluorescence cross sections in the photoexcitation of CH_4, NH_3 and H_2O in the vacuum ultraviolet range2005

    • Author(s)
      N. Kouchi
    • Journal Title

      Atomic and Molecular Data and Their Applications, AIP Conference Proceedings 771

      Pages: 199-208

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] (γ,2γ)experiments for studying the multiply excited states of N_22005

    • Author(s)
      M. Murata, T. Odagiri and N. Kouchi
    • Journal Title

      J. Electron Spectrosc. Relat. Phenom. 144-147

      Pages: 147-149

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Doubly excited states of methane produced by photon and electron interactions2005

    • Author(s)
      H., Fukuzawa, T., Odagiri, T., Nakazato, M., Murata, H., Miyagi, N., Kouchi
    • Journal Title

      Journal of Physics B : Atomic, Molecular and Optical Physics 38(5)

      Pages: 565-578

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Journal Article] Measurements of the fluorescence cross sections in the photoexcitation of CH_4, NH_3 and H_2O in the vacuum ultraviolet range2005

    • Author(s)
      N., Kouchi
    • Journal Title

      Atomic and Molecular Data and Their Applications, AIP Conference Proceedings 771 8

      Pages: 199-20

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Journal Article] (γ, 2γ) experiments for studying the multiply excited states of N_22005

    • Author(s)
      M., Murata, T., Odagiri, N., Kouchi
    • Journal Title

      J. Electron Spectrosc. Relat. Phenom 144-147

      Pages: 147-149

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Journal Article] Doubly excited states of methane produced by photon and electron interactions2005

    • Author(s)
      H.Fukuzawa, T.Odagiri, T.Nakazato, M.Murata, H.Miyagi, N.Kouchi
    • Journal Title

      J.Phys.B : At.Mol.Opt.Phys. 38

      Pages: 565-578

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Measurements of the fluorescence cross sections in the photoexcitation of CH_4,NH_3 and H_2O in the vacuum ultraviolet range2005

    • Author(s)
      Noriyuki Kouchi
    • Journal Title

      AIP CONFERENCE PROCEEDINGS 771

      Pages: 199-208

    • Related Report
      2005 Annual Research Report
  • [Journal Article] (γ,2γ) experiments for studying the multiply excited states of N_22005

    • Author(s)
      Makoto Murata, Takeshi Odagiri, Noriyuki Kouchi
    • Journal Title

      J.Electoron Spectrosc.Relat.Phenom. 144-147

      Pages: 147-149

    • Related Report
      2005 Annual Research Report
  • [Presentation] Multi-electron excitation by photon and electron interactions with molecules2007

    • Author(s)
      T. Odagiri and N. Kouchi
    • Organizer
      ASR 2007, International Symposium on Charged Particle and Photo Interactions with Matter
    • Place of Presentation
      Tokai, Japan
    • Year and Date
      2007-11-06
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Multi-electron excitation by photon and electron interactions witn molecules2007

    • Author(s)
      T., Odagiri, N., Kouchi
    • Organizer
      ASR 2007, International Symposium on Charged Particle and Photon Interactions with Matter
    • Place of Presentation
      Tokai, Japan
    • Year and Date
      2007-11-06
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Multi-electron excitation by photon and electron interactions with molecules2007

    • Author(s)
      T. Odagiri and N. Kouchi
    • Organizer
      7th International Symposium on Advanced Science Research
    • Place of Presentation
      Tokai, Japan
    • Year and Date
      2007-11-06
    • Related Report
      2007 Annual Research Report
  • [Presentation] Doubly excited states of NH_3 as probed by the Lyman-α fluorescence, Acomparison between the electron and photon interactions2007

    • Author(s)
      L. Ishikawa, T. Odagiri, T. Nakazato, M. Kurokawa, K. Yachi, M. Kitajima, and N. Kouchi
    • Organizer
      15th International Symposium on Electron-Molecule Collisions and Swarms
    • Place of Presentation
      Reading, UK
    • Year and Date
      2007-08-03
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Annual Research Report 2007 Final Research Report Summary
  • [Presentation] Doubly excited states of CH_4 as studied by imaging electron-energy-loss spectra tagged with the Lyman-α photons2007

    • Author(s)
      T. Nakazato, T. Odagiri, K. Yachi, L. Ishikawa, H. Fukuzawa, H. Miyagi, M. Kitajima, and N. Kouchi
    • Organizer
      15th International Symposium on Electron-Molecule Collisions and Swarms
    • Place of Presentation
      Reading, UK
    • Year and Date
      2007-08-03
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Annual Research Report 2007 Final Research Report Summary
  • [Presentation] Doubly excited states of NH_3 as probed by the Lyman-α fluorescence, A comparison between the electron and photon interactions2007

    • Author(s)
      L., Ishikawa, T., Odagiri, T., Nakazato, M., Kurokawa, K., Yachi, M., Kitajima, N., Kouchi
    • Organizer
      15th International Symposium on Electron-Molecule Collisions and Swarms
    • Place of Presentation
      Reading, UK
    • Year and Date
      2007-08-03
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Doubly excited states of CH_4 as studied by imaging electron-energy-loss spectra tagged with the Lyman-a photons2007

    • Author(s)
      T., Nakazato, T., Odagiri, K., Yachi, L., Ishikawa, H., Fukuzawa, H., Miyagi, M., Kitajima, N., Kouchi
    • Organizer
      15th International Symposium on Electron-Molecule Collisions and Swarms
    • Place of Presentation
      Reading, UK
    • Year and Date
      2007-08-03
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Theoretical study on the angular correlation of a pair of the Lyman-α photons generated by single-photon absorption of a hydrogen molecule2007

    • Author(s)
      H. Miyagi, A. Ichimura, and N. Kouchi
    • Organizer
      25th International Conference on Photonic, Electronic and Atomic Collisions
    • Place of Presentation
      Freiburg, Germany
    • Year and Date
      2007-07-30
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Annual Research Report 2007 Final Research Report Summary
  • [Presentation] Photon Pair generation from multiply excited states of simple molecules excited by single-photon absorption2007

    • Author(s)
      T. Odagiri, M. Murata, K. Funatsu, T. Tanabe, I. H. Suuki, M. Kitajima, and N. Kouchi
    • Organizer
      25th International Conference on Photonic, Electronic and Atomic Collisions
    • Place of Presentation
      Freiburg, Germany
    • Year and Date
      2007-07-30
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Photon Pair generation from multiply excited states of simple molecules excited by single-photon absorption2007

    • Author(s)
      T. Odagiri, M. Murata, K. Funatsu, T. Tanabe, I.H. Suzuki, M. Kitajima, and N. Kouchi
    • Organizer
      25th International Conference on Photonic, Electronic and atomic Collisions
    • Place of Presentation
      Freiburg, Germany
    • Year and Date
      2007-07-30
    • Related Report
      2007 Annual Research Report
  • [Presentation] Superexcited ammonia produced by photon and electron interactions2007

    • Author(s)
      L. Ishikawa, T. Odagiri, T. Nakazato, M. Kurokawa, K. Yachi, M. Kitajima, and N. Kouchi
    • Organizer
      25th International Conference on Photonic, Electronic and Atomic Collisions
    • Place of Presentation
      Freiburg, Germany
    • Year and Date
      2007-07-27
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Superexcited ammonia produced by photon and electron interactions2007

    • Author(s)
      L. Ishikawa, T. Odagiri, T. Nakazato, M. Kurokawa, K. Yachi, M. Kitajima, and N. Kouchi
    • Organizer
      25th International Conference on Photonic, Electronic and atomic Collisions
    • Place of Presentation
      Freiburg, Germany
    • Year and Date
      2007-07-27
    • Related Report
      2007 Annual Research Report
  • [Presentation] Angle-dependent electron-energy-loss spectra of CH_4 tagged with the Lyman-α photons in the range of the doubly excited states2007

    • Author(s)
      T. Nakazato, T. Odagiri, K. Yachi, L. Ishikawa, H. Fukuzawa, H. Miyagi, M. Kitajima, and N. Kouchi
    • Organizer
      25th International Conference on Photonic, Electronic and Atomic Collisions
    • Place of Presentation
      Freiburg, Germany
    • Year and Date
      2007-07-26
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Angle-dependent electron-energy-loss spectra of CH_4 tagged with the Lyman-α photons in the range of the doubly excited states2007

    • Author(s)
      T. Nakazato, T. Odagiri, K. Yachi, L. Ishikawa, H. Fukuzawa, H. Miyagi, M. Kitajima, and N. Kouchi
    • Organizer
      25th International Conference on Photonic, Electronic and atomic Collisions
    • Place of Presentation
      Freiburg, Germany
    • Year and Date
      2007-07-26
    • Related Report
      2007 Annual Research Report
  • [Presentation] Multiply excited molecules produced by photon and electron interactions2006

    • Author(s)
      T. Odagiri and N. Kouchi
    • Organizer
      The first Asian-Pacific Symposium on Radiation Chemistry
    • Place of Presentation
      Shanghai, China
    • Year and Date
      2006-09-20
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] (γ, 2γ)studies on multiply excited states of H_2 and N_2 in the vacuum ultraviolet range2005

    • Author(s)
      T. Odagiri
    • Organizer
      International Symposium on(e, 2e), Double Photoionization and Related Topics, and 13th International Symposium on Polarization and Correlation in Electronic and Atomic Collisions
    • Place of Presentation
      Buenos Aires, Argentina
    • Year and Date
      2005-07-29
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] (Y, 2Y) studies on multiply excited states of H_2 and N_2 in the vacuum ultraviolet range2005

    • Author(s)
      T., Odagiri
    • Organizer
      International Symposium on (e,2e), Double Photoionization and Related Topics, and 13th International Symposium on Polarization and Correlation in Electronic and Atomic Collisions
    • Place of Presentation
      Buenos Aires, Argentina
    • Year and Date
      2005-07-29
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] Doubly excited methane produced by photon and electron interactions2005

    • Author(s)
      H. Fukuzawa, T. Odagiri, T. Nakazato, H. Miyagi and N. Kouchi
    • Organizer
      24th International Conference on Photonic, Electronic and Atomic Collisions
    • Place of Presentation
      Rosario, Argentina
    • Year and Date
      2005-07-25
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] (γ, 2γ)experiments for studying the multiply excited states of H_2 and N_22005

    • Author(s)
      M. Murata, T. Odagiri and N. Kouchi
    • Organizer
      24th International Conference on Photonic, Electronic and Atomic Collisions
    • Place of Presentation
      Rosario, Argentina
    • Year and Date
      2005-07-22
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2007 Final Research Report Summary
  • [Presentation] (Y, 2Y) experiments for studying the multiply excited states of H_2 and N_22005

    • Author(s)
      M., Murata, T., Odagiri, N., Kouchi
    • Organizer
      24th International Conference on Photonic, Electronic and Atomic Collisions
    • Place of Presentation
      Rosario, Argentina
    • Year and Date
      2005-07-22
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2007 Final Research Report Summary

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Published: 2005-04-01   Modified: 2016-04-21  

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