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Reaction Dynamics in Solution Studied by Ultrafast Visible Pump - Far Infrared Probe Technique

Research Project

Project/Area Number 10206207
Research Category

Grant-in-Aid for Scientific Research on Priority Areas (B)

Allocation TypeSingle-year Grants
Research InstitutionKobe University

Principal Investigator

TOMINAGA Keisuke  Kobe University, Molecular Photoscience Research Center, Professor, 分子フォトサイエンス研究センター, 教授 (30202203)

Project Period (FY) 1998 – 2000
Project Status Completed (Fiscal Year 2001)
Budget Amount *help
¥55,900,000 (Direct Cost: ¥55,900,000)
Fiscal Year 2000: ¥4,300,000 (Direct Cost: ¥4,300,000)
Fiscal Year 1999: ¥4,600,000 (Direct Cost: ¥4,600,000)
Fiscal Year 1998: ¥47,000,000 (Direct Cost: ¥47,000,000)
KeywordsCondenced Phase Dynamics / Ulatrafast Spectroscopy / Terahertz Radiation / Far Infrared Spectroscopy / IR Nonlinear Spectroscopy / Two-Dimensional Vibrational Spectroscopy / Vibrational Dephasing / 高出力赤外短パルス / 非線形分光 / 蛋白質 / 低振動スポエクトル / 集団運動 / 超高速レーザ分光 / 溶液内反応 / 超高速分光 / テラヘルツ分光 / 反応ダイミクス / 反応ダイナミクス
Research Abstract

We have developed two new light sources and spectroscopic techniques in the infrared region to investigate the chemical reactions and relaxation phenomena in condensed phases under this project. One is the third order optical nonlinear spectroscopy in the infrared region using intense femtosecond infrared pulses. The infrared pulses are generated by some optical nonlinear processes such as difference frequency mixing and optical parametric generation/amplification. Group velocity dispersion in the pulse is compensated by inserting a silicon plate in the optical path. The pulse width is measured to be 55 fs with an energy of more than microJ/pulse by an autocorrelation method, which is the shortest pulse of the infrared pulse with such a high energy to our knowledge. Using this pulse we have constructed optical systems of nonlinear spectroscopy such as transient grating, 2- and 3-pulse photon echo including frequency-resolved version. The frequency-resolved 3-pulse photon echo is one of … More the two-dimensional vibrational spectroscopies. We have applied these techniques to several vibrational modes such as three-atom ions (OCN^- and SCN^-) in polar solvents, the -N=C=N- antistretching modes of large organic molecules, the C=O stretching modes of metal porphyrines, and the CN stretching modes of cyano-iron complexes. We discuss vibrational dynamics of these modes including vibrational population relaxation, pure vibrational dephasing, dynamical fluctuation and spectral diffusion, inhomogeneity of the transition frequency, and so on. The other technique we have developed is a spectroscopic method using terahertz (THz) radiation. The THz radiation is generated by focusing a femtosecond pulse to a semiconductor wafer and amplified by applying a magnetic field to the wafer. The THz radiation is detected by an electro-optic sampling method. By using spectrometer in the far-infrared region with the THz radiation as a light source, we have measured far-infrared absorption spectra of various kinds of condensed phase systems such as bulk liquids, solutions of charge-transfer complexes, biopolymers, and so on. Especially, far infrared spectra of polypeptides and proteins (cytochrom c) were studied in detail, and we discuss relation between structures of the biopolymers and spectra in the low-frequency region. Less

Report

(4 results)
  • 2001 Final Research Report Summary
  • 2000 Annual Research Report
  • 1999 Annual Research Report
  • 1998 Annual Research Report
  • Research Products

    (30 results)

All Other

All Publications (30 results)

  • [Publications] K.Tominaga: "Spectroscopic Application of THz Radiation Generated by Ulrtafast Pulses-Static Far Infrared Absorption Measurements in Condensed Phases-"Advances in Multi-Photon Processes and Spectroscopy. 14. 317-338 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K.Tominaga: "Electron Transfer Dynamics in the Excited State Studied by Stochastic-Liouville Equation"J.Mol.Liq.. 90(No.1). 287-293 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K.Tominaga: "Investigation of Two-Dimensional Vibrational Spectra by a Diagrammatic Approach"Bull.Chem.Soc.Jpn.. 74(No.2). 279-286 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K.Ohta: "Excited-State Dynamics of all-trans-1,3,5,7-Octatetraene in Solution.Direct Observation of the Internal Conversion from the S_2 to S_1 State and Relaxation Process in the S_1 State"J.Phys.Chem.A. 105(No.16). 3973-3980 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] H.Maekawa: "Generation of 55 fs Mid-IR Pulses with a 300 cm^<-1> Spectral Width and μJ/pulse Energy"Jpn.J.Appl.Phys.. (掲載予定).

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K.Yamamoto: "Far-Infrared Absorption Measurements of Polypeptides and Cytochrome c by THz Radiation"Bull.Chem.Soc.Jpn.. (掲載予定).

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K. Tominaga, H. Ohtake, N. Sarukura, K. Saitow, H. Sasakawa, A. Tamura, I. V. Rubtsov, and K. Yoshihara: ""Spectroscopic Application of THz Radiation Generated by Ulrtafast Pulses - Static Far Infrared Absorption Measurements in Condensed Phases-""Advances in Multi-Photon Processes and Spectroscopy, 14, pp. 317-338 (World Scientific, Singapore). (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K. Tominaga and H. Maekawa: ""Electron Transfer Dynamics in the Excited State Studied by Stochastic-Liouville Equation""J. Mol. Liq.. 90(No. 1). 287-293 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K. Tominaga and H. Maekawa: ""Investigation of Two-Dimensional Vibrational Spectra by a Diagrammatic Approach""Bull. Chem. Soc. Jpn.. 74(No. 2). 279-286 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K. Ohta, Y. Naitoh, K. Tominaga, and K. Yoshihara: ""Excited-State Dynamics of all-trans-1,3,5,7-0ctatetraene in Solution. Direct Observation of the Internal Conversion from the S_2 to S_1 State and Relaxation Process in the S_1 State""J. Phys. Chem. A.. 105(No. 16). 3973-3980 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] H. Maekawa, K. Tominaga, and D. Podenas: ""Generation of 55 fs Mid-IR Pulses with a 300 cm^<-1> Spectral Width and μJ/pulse Energy""Jpn. J. Appl. Phys.. (in press).

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K. Yamamoto, K. Tominaga, H. Sasakawa, A. Tanumra, H. Murakami, H. Ohtake, and N. Sarukura: ""Far-Infrared Absorption Measurements of Polypeptides and Cytochrome c by THz Radiation""Bull. Chem. Soc. Jpn. (Special Issue on Time-Resolved Vibrational Spectroscopy). (in press).

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K.Tominaga: "Development of Two-Dimensional Raman Spectroscopy by Higher-Order Optical Nonlinear Spectroscopy"J.Luminescence. 87-89. 101-104 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] K.Tominaga: "Concentration Dependence of the Fifth-Order Two-Dimensional Raman Signal"J.Chinese Chem.Soc.. 47. 631-635 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] K.Tominaga: "Spectroscopic Application of THz Radiation Generated by Ulrtafast Pulses-Static Far Infrared Absorption Measurements in Condensed Phases-"Advances in Multi-Photon Processes and Spectroscopy. 14. 317-338 (2001)

    • Related Report
      2000 Annual Research Report
  • [Publications] K.Saitow: "Supercritical-Fluid Cell with Devices of Variable Optical Path Length Giving Fringe-Free Terahertz Spectra"Rev.Sci.Instrum. 71. 4061-4064 (2001)

    • Related Report
      2000 Annual Research Report
  • [Publications] K.Tominaga: "Investigation of Two-Dimensional Vibrational Spectra by a Diagrammatic Approach"Bull.Chem.Soc.Jpn.. 74(No.2),. 279-286 (2001)

    • Related Report
      2000 Annual Research Report
  • [Publications] K.Ohta: "Excited-State Dynamics of all-trans-1,3,5,7-Octatetraene in Solution. Direct Observation of the Internal Conversion from the S_2 to S_1 State and Relaxation Process in the S_1 State ""J.Phys.Chem.,. (in press).

    • Related Report
      2000 Annual Research Report
  • [Publications] K. Tominaga: "Recent Development of Nonlinear Spectroscopy in liquids"Laser chemistry. 19. 117-122 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] K. Ohata: "Femtosecond Time-resolved Fluorescence Studies of a Dye Molecule in Solution: Ultrafast Relavation Process from a Higher *****"Chemical Physics. 242. 103-114 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] H. Pal: "Ultrafont Intermolecular Electron Transfer from Orthomethoxyaniline to Excited Coumarin Dyes"Journal of Chemical Physics. 110. 11454-11465 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] K. Tominaga: "Stochastic-Liourille Approach to Optically-Induced Electron Transfer: Electronic Coherence in the Reaction Dynamics"Journal of Raman Speetroscopy. 31. 137-144 (2000)

    • Related Report
      1999 Annual Research Report
  • [Publications] K. Tominaga: "Development of Two-Dimensional Raman Spectroscopy by Higher-Order Optical Nonlinear Spectroscopy"Journal of Luminescence. (in press).

    • Related Report
      1999 Annual Research Report
  • [Publications] K. Tominaga: "Concentration Dependence of the Fifth-Order Two-Dimensional Raman Signal"Journal of Chinese Chemical Society. (in press).

    • Related Report
      1999 Annual Research Report
  • [Publications] T.J.Kang: "Femtosccond Relavation of Higher Electronic Eycted State of coumarin in Solution" Chem.Phys Lett.287,1/2. 29-34 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] H.Shirota,: "Substituent Effect and Dusterium isotope Effect of Ultrafast Intermolecular Electron Transfer : coumarin in Electron Donating Solvent" J.Phys.Chem.A.102,18. 3089-3102 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] K.Tominaga: "Overtone Vibrational Dephasing of Chloroform Studied by Higher-Order Nonlinear Spectroscopy" J.Phys.Chem.A. 102,23. 4222-4228 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] H.Shirota: "Ultrafast Intermolecular Electron Transfer in Coumarin-Hydrazine System" Chem.Phys.236. 355-364 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] 富永圭介: "高次非線形分光" 分光研究. 47・2. 93-105 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] 富永圭介: "二次元ラマン分光の新展開" 光化学. (in press).

    • Related Report
      1998 Annual Research Report

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Published: 1998-04-01   Modified: 2016-04-21  

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