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Coherent Photochemical Reactions in Sequential Molecular Systems-Measurement and Theoretical Formulation

Research Project

Project/Area Number 11223203
Research Category

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

Allocation TypeSingle-year Grants
Review Section Science and Engineering
Research InstitutionHOKKAIDO UNIVERSITY

Principal Investigator

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

Co-Investigator(Kenkyū-buntansha) SATO Shin-ichiro  Hokkaido Univ., Grad. School of Eng., Assoc. Prof., 大学院・工学研究科, 助教授 (10262601)
OHTA Nobuhiro  Hokkaido Univ., Res. Inst. Electronic Sci., Prof., 電子科学研究所, 教授 (70113529)
SUMI Hitoshi  Univ. Tsukuba., Inst. of Materials Science, Prof., 大学院・物質工学系, 教授 (10134206)
AKIMOTO Seiji  Hokkaido Univ., Grad. School of Eng., Inst., 大学院・工学研究科, 助手 (40250477)
NISHIMURA Yoshinobu  Hokkaido Univ., Grad. School of Eng., Inst., 大学院・工学研究科, 助手 (60218211)
Project Period (FY) 1999 – 2001
Project Status Completed (Fiscal Year 2001)
Budget Amount *help
¥59,300,000 (Direct Cost: ¥59,300,000)
Fiscal Year 2001: ¥4,800,000 (Direct Cost: ¥4,800,000)
Fiscal Year 2000: ¥8,900,000 (Direct Cost: ¥8,900,000)
Fiscal Year 1999: ¥45,600,000 (Direct Cost: ¥45,600,000)
KeywordsMolecular assemblies / Coherent reaction / Supramolecules / Femtosecond fluorescence / Quantum interference / Photosynthesis / 分子配列系光化学 / コヒーレント光化学 / 超分子 / フェムト秒蛍光分光 / 光合成反応中心 / フェムト秒レーザー
Research Abstract

The Coherent nature of photochemical reaction has been established for highly organized molecular systems through the experimental mesurement and theoretical formulation. The results are summarized as follows.
(1) The first observation of quantum beat signal has been attained for cyclic motion of exciton between two chromophores inanthracene dimers and perylene dimers. This means that the exciton moves coherently back and forth between the two chromophores, and that the photochemical reaction in molecular systems occurs coherently in several ps before the electronic decoherence. A special apparatus was constructed which was capable of quantum-interference control of the reaction.
(2) The coherent photochemical reaction under external electric field was investigated, and found that the reaction was controlled by applying electric field. Several types of porphyrin arrays of 1D (Osuka compounds) exhibited a significant enhancement of conductivity upon photoexcitation. These molecular systems may function as molecular wires switchable by photo-irradiation.
(3) The theoretical formulation has been established for coherent transports of electron and exciton in photosynthetic reaction centers (RC) in plants A higher-order perturbation theory was applied to the cyclic and sequential arrangements of molecules inside the RC proteins.
In Summary, the present reserch project has attained 90% success for the reserch program that we planned initially.

Report

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

    (34 results)

All Other

All Publications (34 results)

  • [Publications] I.Yamazaki: "Oscillatory excitation energy transfer in dithiaanthracenophane Quantum beat in coherent photochemical reaction"J.Phys.Chem.A. 106. 1017-1024 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] S.Akimoto: "Ultrafast excitation transfer and excitation delocalization in linear and crossed-linear arrays of porphyrin dimers"Pure & Appl.Chem.. 71. 2107-2115 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] I.Yamazaki: "Ultrafast energy relaxation and excitation delocalization in excited states of zinc porphyrin dimers and trimers"Acta Phys.Polonica A. 95. 105-120 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] H.Sumi: "Unified theory on rates for electron transfer mediated by a midway molecules,bridging between superexhange processes"J.Phys.Chem.B. 105. 9603-9622 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] N.Chta: "Photoinduced charge transfer along a meso,meso-linked porphyrin array"J.Phys.Chem.B. 103. 11242-11245 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] N.Ohta: "External electric field effects on photoinduced electron transfer between cyanine dye and viologen"Z.Phys.Chem.,Bd.. 213. S191-197 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] I.Yamazaki: "Functionality of Molecular Systems,Vol.2"Springer-Verlag. 244 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] I. Yamazaki: "Oscillatory excitation transfer in dithiaanthracenophane Quantum beat in coherent photochemical process in solution"J. Phys. Chem. A.. 106. 1017-1024 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] S. Akimoto: "Ultrafast excitation transfer and excitation delocalization in linear and crossed-linear arrays of porphyrin dimers"Pure & Appl. Chem.. 71. 2107-2115 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] I. Yamazaki: "Ultrafast energy relaxation and excitation delocalization in excited states of zinc porphyrin dimers and trimers"Acta Phys. Polonica A.. 95. 105-120 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] H. Sumi: "Unified theory on rates for electron transfer mediated by a midway molecules, bridging between superexchange processes"J. Phys. Chem. B. 105. 9603-9622 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] N. Ohta: "Photoinduced charge transfer along a meso, meso-linked porphyrin array"J. Phys. Chem. B. 103. 11242-11245 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] N. Ohta: "External electric field effects on photoinduced electron transfer between cyanine dye and viologen sequential processes"Z. Phys. Chem. Bd.. 213. S191-197 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] I. Yamazaki: "Functionality of molecular systems - Vol. 2"Springer Verlag. 244 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] I.Yamazaki: "Oscillatory excitation transfer in dithiaanthracenophane Quantum beat in coherent phtochemical processes in"J.Phys.Chem.A.. 106. 1017-1024 (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] A.Nakano: "Intramolecular energy transfer in S1 and S2 states of porphyrin trimers"J.Phys.Chem.A.. 105. 4822-4833 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] H.Kawaba: "Electric field effects on fluorescenceof methylene-linked compounds of phenanthrene and N, N-dimethylaniline"J.Phys.Chem.A.. 105. 10261-10270 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] H.Sumi: "Unified theory on rates for electron transfer mediated by midway molecule bridging between superexchange and"J.Phys.Chem.B.. 105. 9603-9622 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] H.Sumi: "Bacterial photosynthesis begins with quantum mechanica coherence"Chem.Rec.. 1. 480-493 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] H.Kawabata: "Evidence for electric field-assisted back-electron transfer through methylene bond in a linked compound"J.Chem.Phys.. 114. 7723-7726 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] H.Imahori,H.Norieda,N. Kat I.Yamazaki,Y.Sakata: "Chain length effect on the structure and photoelectrodhemical properties of self-assembled monolayers."J.Phys.Chem.B.. 104. 1253-1260 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] H.Imahori,H.Yamada,I.Yamazaki,Y.Nishimura: "Vectorial multistep electron transfer at the gold ±electrodes modified with selfassembled monolayers"J.Phys.Chem.B.. 104. 2099-2108 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] N.Ohta,S.Umeuchi,K.Akita I.Nishimura,I.Yamazaki: "Electric field effects on fluorescence of pyrene ina homoheneously distributed system and in an oriented"J.Luminesc.. 87-89. 733-735 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] S.Akimoto,T.Yamazaki,A.Osuka I.Yamazaki,A.Nakano: "Ultrafast excitation transfer and relaxation in linear and crossed-klnear arrays of porphyrins"Pure and Appl.Chem.. 71. 2107-2115 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Y.Nishimura,A.Yasuda,S.Speiser,I.Yamazaki: "Time-resolved analysis of intramolecular electronic enerqy transfer in methylenes-linked naphthalene-"Chem.Phys.Lett.. 323. 117-124 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] H.Sumi: "Structural sterategies in the antenna system of photosynthetic system on the basis of quantum mechanics."

    • Related Report
      2000 Annual Research Report
  • [Publications] 山崎巌: "バイオミメティックスハンドブック(第4章 生体エネルギー論)"エヌ・ティー・エス. 912 (2000)

    • Related Report
      2000 Annual Research Report
  • [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] M.H.Wall, S.Akimoto, 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] N.Ohta, Y.Iwaki, I.Yamazaki, A.Osuka: "Photoinduced charge transfer along a meso, meso-linked porphyrin array"J. Phys. Chem. B. 103. 11242-11245 (1999)

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

    • Related Report
      1999 Annual Research Report
  • [Publications] K.Mukai, S.Abe, H.Sumi: "Theory of rapid excitation-energy tranfer from B800 to optically-forbidden exciton states of B850 in antenna"J. Phys. Chem. B. 103. 6096-6120 (1999)

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

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

    • Related Report
      1999 Annual Research Report

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Published: 1999-04-01   Modified: 2018-03-28  

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