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Ultrafast Spectroscopic Study of Photochemical Dynamics in Solution and Microscopic Environments

Research Project

Project/Area Number 11640521
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeSingle-year Grants
Section一般
Research Field Physical chemistry
Research InstitutionOkazaki National Research Institutes

Principal Investigator

TAHARA Tahei  Institute for Molecular Science, Okazaki National Research Institutes Associate professor, 分子科学研究所, 助教授 (60217164)

Co-Investigator(Kenkyū-buntansha) TAKEUCHI Takeuchi  Institute for Molecular Science, Okazaki National Research Institutes Research Associate, 分子科学研究所, 助手 (50280582)
Project Period (FY) 1999 – 2000
Project Status Completed (Fiscal Year 2000)
Budget Amount *help
¥4,000,000 (Direct Cost: ¥4,000,000)
Fiscal Year 2000: ¥1,100,000 (Direct Cost: ¥1,100,000)
Fiscal Year 1999: ¥2,900,000 (Direct Cost: ¥2,900,000)
Keywordsultrafast spectroscopy / femtosecond / relaxation / photochemistry / time-resolved spectroscopy / coherence / reaction dynamics / condensed phase / ダイナミクス / 光異性化 / 電子緩和
Research Abstract

We studied picosecond and femtosecond dynamics of fundamental molecules in sondensed phase using time-resolved vibrational, electronic spectroscopy both in the time and frequency domain. The major outcome of this research project is summarized as follows.
1. We constructed a non-colinear OPA system that generates sub-10 fs optical pulses. Using the ultrashort optical pulse, we carried out pump-probe experiments for S_1 trans-stilbene, and observed beating signals due to the vibrational coherence (V_<25> mode) in the S_1 state.
2. We investigated the vibronic relaxation process of polyatomic molecules in solution, taking tetrace ne as an example. We succeeded in measuring both S_2 and S_1 time-resolved fluorescence, and clarified the electronic relaxation, IVR, vibrational cooling and rotational diffusion process which successively occur after S_2←S_1 photoexcitation.
3. We studied photoisomerization of azobenzene by picosecond Raman and femtosecond fluorescence spectroscopy. The obtained data directly showed that the S_2 state is almost exclusively relaxed to the 'planar' S_1 state. It means that the 'long-time believed' rotational isomerization pathway in the S_2 state does not exist, and that isomerization after S_2 excitation takes place in S_1 state after electronic relaxation.
4. We investigated ultrafast intramolecular proton transfer of 1,8-dihydroxyanthraquinone, and found that tautomer-type fluorescence appears within 50 fs, which mean that proton translocation takes place within 50 fs in the excited state of this molecule.

Report

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

    (22 results)

All Other

All Publications (22 results)

  • [Publications] N.Sarkar et al.: "Vibronic relaxation of Polyatomic molecules in non-polar solvent : femtosecond anisotropy/intensity measurements of the Sn and S1 fluorescence of tetracene"Journal of Physical Chemistry A. 103. 4808-4814 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] S.C.Jeoung et al.: "Ultrafast decay dynamics of photoexcited Cu(II)(TMpy-P4) in water solvent"Chemical Physics Letters. 309. 369-376 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] T.Tahara et al.: "Femtosecond material response probed by phase-stabilized optical heterodyne detected impulsive stimulated Raman scattering"Laser Chemistry. 19. 149-152 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] S.Y.Arzhantsev et al.: "Ultrafast excited-state proton transfer dynamics of 1, 8-dihydroxyanthraquinone (chrysazin) studied by femtosecond time-resolved fluorescence spectroscopy"Chemical Physic Letters. 330. 83-90 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] S.Takeuchi et al.: "Vibrational coherence of S_1 trans-stilbene in solution observed by 40-fs-resolved absorption spectroscopy : Comparison of the low-frequency vibration appearing in the frequency-domain and time-domain spectroscopies"Chemical Physic Letters. 326. 430-438 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] T.Fujino et al.: "Picosecond time-resolved Raman study of trans-azobenzene"Journal Physical Chemistry A. 104. 4203-4210 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] A.Shimojima et al.: "Picosecond time-resolved resonance Raman study of photoisomerization of retinal"Journal Physical Chemistry B. 104. 9288-9300 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] N.Sarkar et al.: "Vibronic relaxation at Polyatomic molecules in non-polar solvent : femtosecond anisotropy / intensity measurements of the Sn and S1 fluorescence of tetracene"J.Phys.Chem.A. 103. 4808-4814 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] S.C.Jeoung et al.: "Ultrafast decay dynamics of photoexcited Cu (II)(TMpy-P4) in water solvent"Chem.Phy.Lett.. 309. 369-376 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] T.Tahara et al.: "Femtosecond material response probed by phase-stabilized optical heterodyne detected impulsive stimulated Raman scattering"Laser Chem.. 19. 149-152 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] S.Arzhantsev et al.: "Ultrafast excited-state proton transfer dynamics of 1,8-dihydroxyanthraquinone (chrysazin) studied by femtosecond time-resolved fluorescence spectroscopy"Chem.Phys.Lett.. 330. 83-90 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] S.Takeuchi et al.: "Vibrational coherence of S_1 trans-stilbene in solution observed by 40-fs-resolved absorption spectroscopy : Comparison of the low-frequency vibration appearing in the frequency-domain and time-domain spectroscopies"Chem.Phys.Lett.. 326. 430-438 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] T.Fujino et al.: "Picosecond time-resolved Raman study of trans-azobenzene"J.Phys.Chem.A. 104. 4203-4210 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] A.Shimojima et al.: "Picosecond time-resolved resonance Raman study of photoisomerization of retinal"J.Phys.Chem.B. 104. 9288-9300 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Sergei Y.Arzhantsev et al.: "Ultrafast excited-state proton transfer dynamics of 1,8-dihydroxyanthraquinone (chrysazin) studied by femtosecond time-resolved fluorescence spectroscopy"Chemical Physic Letters. 330. 83-90 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] S.Takeuchi et al.: "Vibrational coherence of S_1 trans-stilbene in solution observed by 40-fs-resolved absorption spectroscopy : Comparison of the low-frequency vibration appearing in the frequency-domain and time-domain spectroscopies"Chemical Physic Letters. 326. 430-438 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] T.Fujino et al.: "Picosecond time-resolved Raman study of trans-azobenzene"Journal Physical Chemistry A. 104. 4203-4210 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] A.Shimojima et al.: "Picosecond time-resolved resonance Raman study of photoisomerization of retinal"Journal Physical Chemistry B. 104. 9288-9300 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] N Sarkar et al.: "Vibronic Relaxation of Polyatomic Molecule in Non-polar Solvent : Femtosecond Anisotropy/Intensity Measurements of the S_n and S_1 Flicorescence of Tetracene"Journal of Physical Chemistry A. 103. 4808-4814 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] S. C. Jeoung et al.: "Ultrafast Decay Dynamics of Photoexcited Cu(II)(TMpy-P4) in Water Solvent"Chemical Physics Letters. 309. 369-376 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] T. Tahara et al.: "Femtosecond Material Response Probed by Phase-Stabilized Optical Heterodyne Detected Impulsive Stimulated Roman Scattering"Laser Chemistry. 19. 149-152 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] T. Fujino et al.: "Picosecond Time-Resolved Roman Study of Trans-Azobenzene"Journal of Physical Chemistry A. (印刷中).

    • Related Report
      1999 Annual Research Report

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

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