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Sequential photochemical processes in biological and artificial molecular systems

Research Project

Project/Area Number 09304056
Research Category

Grant-in-Aid for Scientific Research (A)

Allocation TypeSingle-year Grants
Section一般
Research Field Physical chemistry
Research InstitutionHOKKAIDO UNIVERSITY

Principal Investigator

YAMAZAKI Iwao  Grad. School of Eng., Hokkaido Univ., Pro., 大学院・工学研究科, 教授 (80002111)

Co-Investigator(Kenkyū-buntansha) AKIMOTO Seiji  Grad. School of Eng., Hokkaido Univ., Asso. Pro., 大学院・工学研究科, 助手 (40250477)
NISHIMURA Yoshinobu  Grad. School of Eng., Hokkaido Univ., Asso. Pro., 大学院・工学研究科, 助手 (60218211)
OHTA Nobuhiro  Research Institute for Electronic Science, Hokkaido Univ., Pro., 電子科学研究所, 教授 (70113529)
MIMURO Mamoru  Faculty of Sci., Yamaguchi Univ., Pro., 理学部, 教授 (40142004)
OSUKA Atsuhiro  Grad. School of Sci., Kyoto Univ., Pro., 理学研究科, 教授 (80127886)
Project Period (FY) 1997 – 1999
Project Status Completed (Fiscal Year 1999)
Budget Amount *help
¥30,100,000 (Direct Cost: ¥30,100,000)
Fiscal Year 1999: ¥1,700,000 (Direct Cost: ¥1,700,000)
Fiscal Year 1998: ¥8,300,000 (Direct Cost: ¥8,300,000)
Fiscal Year 1997: ¥20,100,000 (Direct Cost: ¥20,100,000)
KeywordsOrganized molecular systems / Electron transfer / Excitation transfer / Femtosecond laser / Photosynthesis / Porphyrins / 分子配列システム / フェムト秒時間分解蛍光 / LB膜
Research Abstract

This research project aims at presenting a new aspect of photochemical processes in highly organized molecular systems in which reacting molecules are located with close proximity and optimal orientation. The reaction dynamics of ultrafast and non-equilibrium processes in electron transfer and excitation transfer were monitored with femtosecond time-resolved fluorescence spectroscopy. The result of this study is summarized in the following. (1) In Langmuir-Blodgett multilayers, it was found that the inter- and intra-layer excitation transfer took place much faster at room temperature (ca. 10 ps) than in 10K (ca. 50 ps). The theoretical analyses suggest that the spatical fluctuation of molecules may play an important role in excitation transfer. (2) In artificial porphyrin arrays and photosynthetic carotenoid-chlorophyll systems, the excitation energy transfer occurs directrly from the donor S2 state during 80-140 fs before thermal equilibration. This finding violates the well-known Kasha's rule that the photochemical reaction proceeds from the thermally equilibrated lowest excited state. (3) External electric field effect It was found that the electron transfer in LB films undergoes the external electrid field and its reaction rate depend stronly on the initially excited state. The results of the project are now directed toward development of quantum computing elecments and photo-switching molecular devices.

Report

(4 results)
  • 1999 Annual Research Report   Final Research Report Summary
  • 1998 Annual Research Report
  • 1997 Annual Research Report
  • Research Products

    (35 results)

All Other

All Publications (35 results)

  • [Publications] I.YAMAZAKI,S.Akimoto,H.Shiratori,A.Osuka: "Ultrafast energy relaxation and excitation delocalzation in excited states of zinc porphyrin dimers"Acta Phys.Polonica A. 95. 105-120 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] A.Osuka,M.Ikeda,H.Shiratori,Y.Nishimura,I.Yamazaki: "Accelerated singlet energy transfer in bis(phenyl)-phenylene-bridged 5,10,15,20-tetraaryl zinc-free"J.Chem.Soc.Perkin Trans.. 2. 1019-1025 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] M.Mimuro,S.Akimoto,I.Yamazaki,H.Miyashita,S.Miyachi: "Fluorescence properties of chlorophyll d-dominating prokaryoteic alga, Acaryochloris marina"Biochim.Biophys.Acta. 1412. 37-46 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] M.H.Wall,S.Akimoto,N.Ohta,I.Yamazaki,H.Kido: "Ultrafast intramolecular electron transfer in peripherally ruthenated zinc tetraarylporphyrins"Bull.Chem.Soc.Jpn.. 72. 1475-1481 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] S.Akimoto,T.Yamazaki,I.Yamazaki,A.osuka: "Excitation relaxation of zinc and free-base porphyrin probed by femtosecond fluorescence spectroscopy"Chem.Phys.Lett.. 309. 177-182 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] I.Yamazaki,M.Yamaguchi,S.Akimoto,N.Ohta: "Non-equilibrium excitation energy transfer in sequentially stacking molecular systems"J.Liminescence. 72/73. 71-74 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] I.Yamazaki: "Functionality of Molecular Systems-From Molecular Systems to Molecular Devices, Vol2"Springer Verlag-Tokyo. 245 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] I. Yamazaki, S. Akimoto, H. Shiratori, A. Osuka: "Ultrafast energy relaxation and excitation delocalization in excited states of zinc porphyrin dimers and trimer"Acta. Phys. Polonica A. 95. 105-120 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] A. Osuka, M. Ikeda, H. Shiratori, Y. Nishimura, I. Yamazaki: "Accelerated singlet energy transfer in bis(phenyl)-phenylene-bridged 5,10,15,20-tetraaryl zinc-free base hybrid diporphyrins"J. Chem. Soc. Perkin Trans.. 2. 1019-1025 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] M. Mimuro, S. Akimoto, I. Yamazaki, H. Miyashita: "Fluorescence propeerties of chlorophyll d-dominating prokaryoteic alga. Acarvochloris marina"Biochim. Biophys. Acta. 1412. 37-46 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] M. H. Wall, S. Akimoto, N. Ohta, I. Yamazaki, H. Kid: "Ultrafast intramolecular electron transfer in peripherally ruthenated zinc tetraarylporphyrins."Bull. Chem. Soc. Jpn.. 72. 1475-1481 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] S. Akimoto, T. Yamazaki, I. Yamazaki, A. Osuka: "Excitation relaxation of zinc and free-base porphyrin probed by femtosecond fluorescence spectroscopy."Chem. Phys. Lett.. 309. 177-182 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] I. Yamazaki, M. Yamaguchi, S. Akimoto, N. Ohta: "Non-equilibrium excitation energy transfer in sequentially stacking molecular systems."J. Luminescence. 72/73. 71-74 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] I. Yamazaki: "Functionality of Molecular Systems. Vol. 2"Springer-Verlat, Tokyo. Total pages 245 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] I. YAMAZAKI, S. Akimoto, H. Shiratori, A. Osuka: "Ultrafast energy relaxation and excitation delocalization in excited states of zinc porphyrin dimers"Acta Phys. Polonica A. 95. 105-120 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] A. Osuka, M. Ikeda, H. Shiratori, Y. Nishimura, I. Yamazaki: "Accelerated singlet energy transfer in bis(phenyl)-phenylene-bridged 5,10,15,20-tetraaryl zinc-free"J. Chem. Soc. Perkin Trans.. 2. 1019-1025 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] M. Mimuro, S. Akimoto, I. Yamazaki, H. Miyashita, S. Miyachi: "Fluorescence properties of chlorophyll d-dominating prokaryoteic alga, Acaryochloris marina"Biochim. Biophys. Acta. 1412. 37-46 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] M. H. Wall, S. Akimoto, N. Ohta, I. Yamazaki, H. Kido: "Ultrafast intramolecular electron transfer in peripherally ruthenated zinc tetraarylporphyrins"Bull. Chem. Soc. Jpn.. 72. 1475-1481 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] S. Akimoto, T. Yamazaki, I. Yamazaki, A. Osuka: "Excitation relaxation of zinc and free-base porphyrin probed by femtosecond fluorescence spectroscopy"Chem. Phys. Lett.. 309. 177-182 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] I. Yamazaki, M. Yamaguchi, S. Akimoto, N. Ohta: "Non-equilibrium excitation energy transfer in sequentially stacking molecular systems"J. Liminescence. 72/73. 71-74 (1997)

    • Related Report
      1999 Annual Research Report
  • [Publications] I. Yamazaki: "Functionality of Molecular Systems-From Molecular Systems to Molecular Devices, Vol. 2"Springer Verlag-Tokyo. 245 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] I.Yamazaki, S.Akimoto, A.Osuka, H.Shiratori: "Ultrafast energy relaxation and excitation delocalization in excuted states of Zinc porphyrin dimers and trimer" Acta Phys.Polonica A. 95. 105-120 (1999)

    • Related Report
      1998 Annual Research Report
  • [Publications] S.Abe, Y.Nishimura, I.Yamazaki, N.Ohta: "Remarkable electric field effect on the absorption intensity of a molecular aggregate of photomerocyanine in aPMMA film" Chem.Lett.1999. 165-166 (1999)

    • Related Report
      1998 Annual Research Report
  • [Publications] N.Ohta, S.Umeuchi, Y.Nishimura, I.Yamazaki: "Electric-field induced quenching of exciplex fluorescence and photocurrent generation in a mixture of ethylcarbazole" J.Phys.Chem.102. 3784-3790 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] N.Ohta, T.Kanada, I.Yamazaki, M.Ito: "External electric field effects on the fluorescence of methy-lene-linked pyrene and N,N-dimethylaniline in PMMA films" Chem.Phys.Lett.292. 535-541 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] M.Mimuro, M.Watanabe, M.Tokutomi I.Yamazaki: "Multiple pathways of excitation energy flow in the photo-synthetic pigment system of a cryptophyte,cryptomonas sp." Phycological Rep.46. 155-164 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] A.Nakano, A.Osuka, ± I.Yamazaki, N.Nishimura: "Windmill-like porphyrin arrays as potent light-harvesting antenna complexes" Angew.Chem.Int.Ed.37. 3023-3027 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] I.Ymazaki: "Functionality of Molecular Systems Vol.2" Springer-Verlag Tokyo, 245 (1999)

    • Related Report
      1998 Annual Research Report
  • [Publications] I.Yamazaki, S.Akimoto N.Ohta: "Non-equilibrium excitation energy transfer in sequential stacking molecular systems" J.Luminescence. 72/74. 71-74 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] N.Ohta, T.Nomura I.Yamazaki: "External electrifield effect on photoinduced interlayer electron transfer in LB films" J.Photochem.Photobiol. 106. 37-43 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] M.Mimuro, S.Akimoto, I.Yamazaki: "Effect of molecular structures and solvents on the excited state dynamics of the S2 state of carotenoids" J.Am.Chem.Soc.119. 1452-1453 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] N.Ohta, M.Koizumi, Y.Nishimura, I.Yamazaki: "External electric field effects on fluorescence in an electron donor and acceptor system" J.Phys.Chem.100. 16466-16471 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] 山崎 巌, 大須賀篤弘, 三室 守, 太田信廣: "分子系超構造における光量子ダイナミクス-光合成系から分子コンピューターへ" 表面. 35. 418-424 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] 三室 守, 山崎 巌: "光エネルギーを運ぶ分子配列によるハイウエーの設計" 化学と工業. 50. 713-716 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] 山崎 巌: "光コンピューティングの事典" 朝倉書店, 534 (1997)

    • Related Report
      1997 Annual Research Report

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Published: 1997-04-01   Modified: 2016-04-21  

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