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Development of Various Two-Dimensional Vibrational Spectroscopy and Its Application for Practical Use

Research Project

Project/Area Number 13554019
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section展開研究
Research Field Physical chemistry
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)

Co-Investigator(Kenkyū-buntansha) NISHIZAWA Seiji  Japan Science and Technology Agency, Project Leader, 時系列変換パルス分光計測システム, 研究開発リーダ(研究職)
Project Period (FY) 2001 – 2003
Project Status Completed (Fiscal Year 2003)
Budget Amount *help
¥14,000,000 (Direct Cost: ¥14,000,000)
Fiscal Year 2003: ¥4,000,000 (Direct Cost: ¥4,000,000)
Fiscal Year 2002: ¥4,800,000 (Direct Cost: ¥4,800,000)
Fiscal Year 2001: ¥5,200,000 (Direct Cost: ¥5,200,000)
Keywords2D Vibrational Spectroscopy / IR Photon Echo / IR Transient Grating / IR Short Pulse / Femtosecond Solid State Laser / Anharmonicity / Vibrational Dephasing / Vibrational Population Relaxation / 赤外非線形分光
Research Abstract

By using a infrared short pulse with a duration of 55 fs and energy more than 1 μJ/pulse, which is the shortest IR pulse with a high energy, we have developed third order optical nonlinear spectroscopy and applied to vibrational dynamics in condensed phases. The examples are three-pulse photon echo method, wavelength-resolved three-pulse photon echo method, and wavelength-resolved transient grating method. In these methods we can plot a signal as a function of multi-dimensional coordinates such as delay time and frequency. Especially, wavelength-resolved three-pulse photon echo method is a vibrational analogue of two-dimensional NMR. We applied these methods to several vibrational modes in condensed phases to obtain, for example, the time-correlation function of the transition frequency fluctuation, lifetime of the vibrational excited state, reorientational time, and anharmonicity. The examples are the anti-symmetric stretching modes of OCN^-and SCN^-in methanol, the anti-symmetric CN … More stretching mode of Fe(CN)_6^<4->, the CO stretching mode of coordinated to Ruporphyryine, anti-symmetric -N=C=N-stretching mode, and the OH stretching mode of water in a reverse micelle. One of the problems to be overcome for practical use is to obtain very stable IR pulse. At first, we thought that IR short pulse should have an enough high energy, but we found that rather than that shot-to-shot stability of the pulse is more important that the high energy. The present system uses superfluorescence for optical parametric generation (OPG), and this method easily introduces un-stable nature in the pulse. Therefore, we have constructed a new system which uses white light for OPG, and difference frequency mixing set up to generate IR pulses. We have obtained idler pulses in the near IR region from 1.7 to 2.4 mm, signal pulses in the near IR region from 1.1 to 1.5 mm, and IR pulse in the mid-IR region from 3.0 to 5.0 mm. A shot-to-shot stability of the mid IR pulse is about 0.3%, which is almost the best performance ever recorded. Less

Report

(4 results)
  • 2003 Annual Research Report   Final Research Report Summary
  • 2002 Annual Research Report
  • 2001 Annual Research Report
  • Research Products

    (28 results)

All Other

All Publications (28 results)

  • [Publications] H.Maekawa: "Generation of 55 fs Mid-IR Pulses with a 300cm^<-1> Spectral Width and μJ/pulse energy"Jpn.J.Appl.Phys.. 41. L329-L331 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] K.Ohta: "Probing the Spectral Diffusion of Vibrational Transition of OCN^- and SCN^- in Methanol by Three-Pulse Infrared Photon Echo Specroscopy"J.Phys.Chem.A. 107. 5643-5649 (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] K.Ohta: "Vibrational Population Relaxation and Dephasing Dynamics of Fe(CN)_6^<4-> in D_2O with Third-Order Nonlinear Infrared Spectroscopy"J.Phys.Chem.A. 108. 1333-1341 (2004)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] K.Ohta: "Vibrational Polulation Relaxation and Dephasing Dynamics of Fe(CN)_6^<4-> in Water : Deuterium Isotope Effect of Solvents"Chem.Phys.Lett.. 386. 32-37 (2004)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] K.Ohta: "Vibrational Dynamics in Liquids Studied by Infrared Nonlinear Spectroscopy"Proceedings of TSRP(Trombay Symposium on Radiation & Photochemistry)-2004. 1. 24-27 (2004)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] H.Maekawa: "Vibrational Dynamics of the OH Stretching Mode of Water in Reverse Micelles", Studied by Infrared Nonlinear Spectroscopy"2003 Material Research Society Fall Meeting Symposium Proceedings. 790. 6.7.1-6.7.11 (2004)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] K.Tominaga, H.Maekawa: "Two-Dimensional Optical Nonlinear Spectroscopy in Liquids"Femtochemistry (ed.by F.C.De Schryver, and G.Schweitzer) (Wiley-VCH, Weinheim). IV. 217-223 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] K.Tominaga, 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
      2003 Final Research Report Summary
  • [Publications] H.Maekawa, K.Tominaga, D.Podenas: "Generation of 55 fs Mid-IR Pulses with a 300cm-1 Spectral Width and μJ/pulse Energy"Jpn.J.Appl.Phys.. 41(Part2, No.3b). L329-L331 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] K.Ohta, H.Maekawa, S.Saito, K.Tominaga: "Probing the Spectral Diffusion of Vibrational Transitions of OCN and SCN in Methanol By Three-Pulse Infrared Photon Echo Spectroscopy"J.Phys.Chem.. A107(No.30). 5643-5649 (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] K.Ohta, H.Maekawa, S.Saito, K.Tominaga: "Vibrational Population Relaxation and Dephasing Dynamics of Fe(CN)64-in D20 with Third-Order Nonlinear Infrared Spectroscopy"J.PHYs.Chem.. A108(NO.8). 1333-1341 (2004)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] K.Ohta, H.Maekawa, S.Saito, K.Tominaga: "Vibrational Population Relaxation and Dephasing Dynamics of Fe(CN)64-in Water : Deuterium Isotope Effect of Solvents"J.PHYs.Chem.. A386(NO.1-3). 32-37 (2004)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] K.Ohta, H.Maekawa, S.Saito, K.Tominaga: "Vibrational Dynamics in Liquids Studied by Infrared Nonlinear Spectroscopy"Proceedings of TSRP (Trombay Symposium on Radiation&Photochemistry)-2004. Vol.1. 24 (2004)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] H.Maekawa, K.Ohta, K.Tominaga: "Vibrational Dynamics of OH Stretching Moge of Water in Reverse Micelles "Studied by Infrared Nonlinear Spectroscopy""Materials Research Society Symposium Proceedings (ed.by J.T.Fouekas, Levitz M.Urbakh, and K.J.Wahl). Vol.790. 6.7.1-6.7.11 (2004)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] K.Ohta: "Probing the Spectral Diffusion of Vibrational Transitions of OCN^- and SCN^- in Methanol by Three-Pulse Infrared Photon Echo Spectroscopy"J.Phys.Chem.A. 107(No.30). 5643-5649 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] K.Ohta: "Vibrational Population Relaxation and Dephasing Dynamics of Fe(CN)_6^<4-> in D_2O with Third-Order Nonlinear Infrared Spectroscopy"J.Phys.Chem.A. 108(No.8). 1333-1341 (2004)

    • Related Report
      2003 Annual Research Report
  • [Publications] K.Ohta: "Vibrational Population Relaxation and Dephasing Dynamics of Fe(CN)_6^<4-> in Water : Deuterium Isotope Effect of Solvents"Chem.Phys.Lett.. 386(No.1-3). 32-37 (2004)

    • Related Report
      2003 Annual Research Report
  • [Publications] K.Ohta: "Vibrational Dynamics in Liquids Studied by Infrared Nonlinear Spectroscopy"Proceedings of TSRP (Trombay Symposium on Radiation & Photochemistry)-2004. 1. 24-27 (2004)

    • Related Report
      2003 Annual Research Report
  • [Publications] H.Maekawa: "Vibrational Dynamics of the OH Stretching Mode of Water in Reverse Micelles", Studied by Infrared Nonlinear Spectroscopy"2003 Material Research Society Fall Meeting Symposium Proceedings. (in press).

    • Related Report
      2003 Annual Research Report
  • [Publications] K.Yamamoto: "Far-Infrared Absorption Measurements of Polypeptides and Cytochromec by THz Radiation"Bull. Chem. Soc. Jpn.. 75(No.5). 1083-1092 (2002)

    • Related Report
      2002 Annual Research Report
  • [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. (2002). 41(Part 2,No.3B). L329-L331 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] K.Tominaga: ""Vibrational Dynamics in Porous Silica Glasses Studied by Time-Resolved Coherent Anti-Stokes Raman Scattering", in Liquid Dynamics"American Chemical Society. 160-168 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] K.Tominaga: ""Spectroscopic Application of THz Radiation Generated by Ultrafast Pulses -Static Far Infrared Absorption Measurements in Condensed Phases-""Advances in Multi-Photon Processes and Spectroscopy. 14. 317-338 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Tominaga: ""Electron Transfer Dynamics in the Excited State Studied by Stochastic-Liouville Equation""J. Mol. Liq.. 90(NO.1). 287-293 (2001)

    • Related Report
      2001 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
      2001 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. A. 105(No.16). 3973-3980 (2001)

    • Related Report
      2001 Annual Research Report
  • [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).

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Yamamoto: ""Far-Infrared Absorption Measurements of Polypeptides and Cytochrome c by THz Radiation""Bull. Chem. Soc. Jpn.. (掲載予定).

    • Related Report
      2001 Annual Research Report

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Published: 2001-04-01   Modified: 2016-04-21  

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