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Theoretical study on ultrafast chemical processes in terms of pump-probe photoelectron spectroscopy

Research Project

Project/Area Number 11440170
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

TAKATSUKA Kazuo  The University of Tokyo, Graduate School of Arts and Sciences, Professor, 大学院・総合文化研究科, 教授 (70154797)

Project Period (FY) 1999 – 2001
Project Status Completed (Fiscal Year 2001)
Budget Amount *help
¥14,100,000 (Direct Cost: ¥14,100,000)
Fiscal Year 2001: ¥2,800,000 (Direct Cost: ¥2,800,000)
Fiscal Year 2000: ¥5,300,000 (Direct Cost: ¥5,300,000)
Fiscal Year 1999: ¥6,000,000 (Direct Cost: ¥6,000,000)
Keywordsphotoelectron spectroscopy / wave-packet dynamics / pump-probe spectroscopy / nonadiabatic transition / 超高速ダイナミクス / 量子波束 / 量子波乗
Research Abstract

We have developed a theory of energy- and angle-resolved photoelectron spectra for femtosecond pump-probe ionization of wavepackets and results of its application to the ^1Σ^+_μ double-minimum state of aligned Na_2. The formulation is well suited for inclusion of the underlying dynamics of molecular photoionization and its dependence on molecular geometry. Results have been obtained for three typical pump laser energies selected so as to investigate qualitatively different patterns of the spatio-temporal propagation of wavepackets on the double-minimum potential curve and of their associated photoelectron spectra. Photoelectron angular distributions have been given for different orientations of linearly polarized pump and probe pulses. The resulting photoelectron spectra illustrate the importance of a proper description of the underlying photoionization amplitudes and their dependence on geometry for unravelling wavepacket dynamics from pump-probe photoelectron signals in non-adiabatic regions where the electronic structure evolves rapidly with geometry. The present theory was extended so as to treat a system of nonadiabatic transition such as that in NaI molecule, whose ground and first excited potential curves intersect with each other due to intramolecular electron transfer. It has been shown for the first time that the bifurcation of nuclear wavepackets can be directly and experimentally observed with the pump-probe photoelectron spectroscopy. This is of great importance both in chemistry, wave-pacekt engineering, quantum chaos, the fundamental quantum theory, and so on.

Report

(4 results)
  • 2001 Annual Research Report   Final Research Report Summary
  • 2000 Annual Research Report
  • 1999 Annual Research Report
  • Research Products

    (38 results)

All Other

All Publications (38 results)

  • [Publications] Y.Arasaki, K.Takatsuka, K.Wang, V.McKoy: "Femtosecond Energy-and Angle-Resolved Photoelectron Spectra"Chem. Phys. Lett.. 302. 363-374 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Y.Arasaki, K.Takatsuka, K.Wang, V.McKoy: "Femtosecond Energy-and Angle-Resolved Photoelectron Spectroscopy"J. Chem. Phys.. 112. 8871-8884 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Y.Arasaki, K.Takatsuka, K.Wang, V.McKoy: "Probing Wavepacket Dynamics with Femtosecond Energy-and Angle-Resolved Photoelectron Spectroscopy"J. Electron Spectr. Relat. Phenom.. 108. 89-98 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K.Takatsuka, Y.Arasaki, K.Wang, V.McKoy: "Introductory Lecture. Probing Wavepacket Dynamics with Femtosecond Energy-and Angle-Resolved Photoelectron Spectroscopy"Faraday Discuss. 115. 1-15 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Y.Arasaki, K.Takatsuka, K.Wang, V.McKoy: "Energy-and Angle-Resolved Pump-Probe Photoelectron Spectroscopy : Molecular Rotation"J. Chem. Phys.. 114. 7941-7950 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Y.Arasaki, K.Takatsuka, K.Wang, V.McKoy: "Energy-and angle-resolved femtosecond photoelectron spectra from rotating molecules"Femtochemistry, F.C. De Schryver et al. Ed. Wiley-VCH, New York. (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Y.Arasaki, K.Takatsuka, K.Wang, V.McKoy: "Pump-probe photoionization study of the passage and bifurcation of a quantum wavepacket across an avoided crossing"Physical Review Letters. (submitted for publication). (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Y.Arasaki, K.Takatsuka, K.Wang, V.McKoy: "Studies of electron transfer in NaI with pump-probe femtosecond photoelectron spectroscopy"(In preparation). (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] 高塚 和夫: "非平衡系の科学IV 分子の複雑性とカオス"講談社サイエンティフィク. 182 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Y. Arasaki, K. Takatsuka, K. Wang, and V. McKoy: "Femtosecond Energy- and Angle-Resolved Photoelectron Spectra"Chem. Phys. Lett.. 302. 363-374 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Y. Arasaki, K. Takatsuka, K. Wang, and V. McKoy: "Femtosecond Energy- and Angle-Resolved Photoelectron Spectroscopy"J. Chem. Phys.. 112. 8871-8884 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Y. Arasaki, K. Takatsuka, K. Wang, and V. McKoy: "Probing Wavepacket Dynamics with Femtosecond Energy- and Angle-Resolved Photoelectron Spectroscopy"J. Electron Spectr. Relat. Phenom.. 108. 89-98 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K. Takatsuka, Y. Arasaki, K. Wang, and V. McKoy: "Introductory Lecture. Probing Wavepacket Dynamics with Femtosecond Energy- and Angle-Resolved Photoelectron Spectroscopy"Faraday Discuss.. 115. 1-15 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Y. Arasaki, K. Takatsuka, K. Wang, and V. McKoy: "Energy- and Angle-Resolved Pump-Probe Photoelectron Spectroscopy : Molecular Rotation"J. Chem. Phys.. 114. 7941-7950 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Y. Arasaki, K. Takatsuka, K. Wang, and V. McKoy: "Energy- and angle-resolved femtosecond photoelectron spectra from rotating molecules"Femtochemistry, F.C. De Schryver et al. Ed. Wiley-VCH, New York. (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Y. Arasaki, K. Takatsuka, K. Wang, and V. McKoy: "Pump-probe photoionization study of the passage and bifurcation of a quantum wavepacket across an avoided crossing"Physical Review Letters. submitted for publication. (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Y. Arasaki, K. Takatsuka, K. Wang, and V. McKoy: "Studies of electron transfer in NaI with pump-probe femtosecond photoelectron spectroscopy"in preparation. (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] H.Fujisaki, K.Takatsuka: "Highly Excited Vibronic Eigenfunctions in a Multimode Nonadiabaitic System with Duschinsky Rotation"J. Chem. Phys.. 114. 3497-3507 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Takatsuka: "Variational Statistical Theory for Microcanonical Ensemble and the Linear Surprisal in Chemical Reaction Dynamics"Chem. Phys. Lett.. 345. 453-460 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] H.Ushiyama, T.Arasaki, K.Takatsuka: "Efficient Calculations of Classical Trajectories and Stability Matrices for Semiclassical Theory with Locally Analytic Inegrator. The Hulme"Chem. Phys. Lett.. 346. 169-176 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] Y.Arasaki, K.Takatsuka, K.Wang, V.McKoy: "Energy- and Angle-Resolved Pump-Probe Femtosecond Photoelectron Spectroscopy : Molecular Rotation"J. Chem. Phys.. 114. 7941-7950 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] H.Fujisaki, K.Takatsuka: "Chaos Induced by Quantum Effect Due to Breakdown of the Born-Oppenheimer Nonadiabaticity"Phys. Rev. E. 63. 066221-066231 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Takatsuka: "Amplitude-free Correlation Function Based on an Algebra for Coordinate Transformation in Semiclassical Integrals"Phys. Rev. E.. 64. 016224-016232 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] A.Inoue, Ushiyama, K.Takatsuka: "Semiclassical Quantization of Strongly Chaotic Vibrations in M7-like Cluster"Phys. Rev. E.. 64. 056223-056238 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] H.Ushiyama, K.Takatsuka: "Successive Mechanism of Double Proton Transfer in Formic Acid Dimer. A Classical Study"J. Chem. Phys.. 115. 5903-5912 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] 高塚 和夫: "非平衡系の科学IV 分子の複雑性とカオス"講談杜サイエンティフィク. 182 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] Y.Arasaki,K.Takatsuka,K.Wang,and V.McKoy: "Probing Wavepacket Dynamics with Femtosecond Energy- and Angle-Resolved Photoelectron Spectroscopy."J.Electr.Spec.Rel.Phenom.. 108. 89-98 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Y.Arasaki,K.Takatsuka,K.Wang,and V.McKoy: "Femtosecond Energy- and Angle-resolved Photoelectron Spectroscopy."J.Chem.Phys.. 112. 8871-8884 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Y.Arasaki,K.Takatsuka,K.Wang,and V.McKoy: "Probing Wavepacket Dynamcis with Femtosecond Energy- and Angle-Resolved Photoelectron Spectroscopy."Faraday Discussion, Introductory Lecture. 115. 1-15 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] H.Fujisaki and K.Takatsuka: "Highly Excited Vibrational Eigenfunctions in a Multimode Nonadiabatic System with Duschinsky Roataion."J.Chem.Phys.. 114. 3497-3507 (2001)

    • Related Report
      2000 Annual Research Report
  • [Publications] Y.Arasaki,K.Takatsuka,K.Wang,and V.McKoy: "Energy- and Angle-Resolved Pump-Probe Femtosecond Photoelectron Spectroscopy : Molecular Rotation."J.Chem.Phys.. (in press). (2001)

    • Related Report
      2000 Annual Research Report
  • [Publications] H.Fujisaki and K.Takatsuka: "Chaos Induced by Quantum Effect Due to Breakdown of the Born-Oppenheimer Nonadiabaticity."Phys.Rev.E.. (In press).

    • Related Report
      2000 Annual Research Report
  • [Publications] K.Takatsuka: "Concept of inter-basin mixing"J.Chem.Phys.. 110. 3263-3266 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] A.Inoue-Ushiyama: "Semiclassical theory for Maslov-type wave packet"Phys.Rev.A. 59. 3256-3269 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] A.Inoue-Ushiyama: "Role of phase cancellation removing spurious states"Phys.Rev.A. 60. 112-120 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] K.Takatsuka: "Tunneling paths in multidimensional semiclassical dynamics"Phys.Rept.. 322. 347-417 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] A.Arasaki: "Femtosecond energy-and angle-resolved photoelectron"Chem.Phys.Lett.. 302. 363-374 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] T.Yanao: "Time scale of isomerizations and isotropic inflation"Chem.Phys.Lett.. 313. 633-638 (1999)

    • Related Report
      1999 Annual Research Report

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Published: 1999-04-01   Modified: 2016-04-21  

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