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Study of relaxation kinetics of excited states in carotenoids and energy transfer in photosynthesis

Research Project

Project/Area Number 14340089
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field 固体物性Ⅰ(光物性・半導体・誘電体)
Research InstitutionTohoku University

Principal Investigator

YOSHIZAWA Masayuki  Tohoku University, Graduate School of Science, Associate Professor, 大学院・理学研究科, 助教授 (60183993)

Co-Investigator(Kenkyū-buntansha) HASHIMOTO Hideki  Osaka City University, Graduate School of Science, Professor, 大学院・理学研究科, 教授 (50222211)
Project Period (FY) 2002 – 2004
Project Status Completed (Fiscal Year 2004)
Budget Amount *help
¥13,900,000 (Direct Cost: ¥13,900,000)
Fiscal Year 2004: ¥1,900,000 (Direct Cost: ¥1,900,000)
Fiscal Year 2003: ¥3,600,000 (Direct Cost: ¥3,600,000)
Fiscal Year 2002: ¥8,400,000 (Direct Cost: ¥8,400,000)
Keywordscarotenoid / photosynthesis / energy transfer / femtosecond spectroscopy / reaction center / ultrafast relaxation / vibrational excited state / electroabsorption spectroscopy / β-カロテン / リコペン / 分子構造 / フェムト秒ラマン分光 / 10フェムト秒分光 / ^1B_u^-励起状態 / 共役長
Research Abstract

Carotenoids play important roles in light-harvesting (LH) function of photosynthesis. Light energy is initially absorbed by carotenoid and transferred to bacteriochlorophyll with high efficiency. Ultrafast relaxation kinetics of carotenoids has been investigated systematically. Carotenoids with several conjugation lengths and different structures are prepared for the measurements. Their basic optical properties are measured by stationary absorption, fluorescence, and electroabsorption spectroscopies. Femtosecond time-resolved spectroscopy system has been improved and tunable excitation pulses in visible to near-infrared region are utilized. Femtosecond absorption, Raman, and fluorescence spectroscopies have been done under the same excitation condition to compare the results directly.
Ultrafast phenomena in carotenoids are summarized as follows. At delay times of nearly equal to zero, nonlinear optical responses in a three-level system of the ground state (1^1A_g^-), the lowest opticall … More y allowed excited state (1^1B_u^+), and a highly excited state (n^1A_g^-) are observed in addition to the signal due to the resonant excitation of 1^1B_u^+. After the generation of 1^1B_u^+, the internal conversion to a lower dark state (2^1A_g^-) occurs with the time constant of 0.1〜0.2 ps. Another dark state (1^1B_u^-) is an intermediate state of the relaxation, but it cannot be time-resolved in this research. Redistribution and dissipation of excess vibrational energy take place simultaneously with the internal conversions. However, some vibrational modes have long lifetimes and 2^1A_g^-remains in vibrational excited levels longer than several picoseconds. The vibrational energy affect the relaxation kinetics and slows down the internal conversions.
Preliminary measurement of the LH complex has been done and the experimental system is going to be refined for the study of the vibrational level in the LH complex.
This research reveals the main relaxation kinetics of carotenoids and importance of the vibrational levels in the energy transfer from carotenoids to reaction center of the photosynthesis. Less

Report

(4 results)
  • 2004 Annual Research Report   Final Research Report Summary
  • 2003 Annual Research Report
  • 2002 Annual Research Report
  • Research Products

    (42 results)

All 2005 2004 2003 2002 Other

All Journal Article (30 results) Publications (12 results)

  • [Journal Article] Dynamics of Carotenoids Probed by Femtosecond Absorption, Fluorescence, and Raman Spectroscopy2005

    • Author(s)
      M.Yoshizawa, D.Kosumi, M.Komukai, K.Yanagi, H.Hashimoto
    • Journal Title

      Ultrafast Phenomena XIV, Springer Series in Chemical Physics 79

      Pages: 589-591

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Excitation energy dependence of excited states dynamics in all-trans-carotenes determined by femtosecond absorption and fluorescence spectroscopy2005

    • Author(s)
      D.Kosumi, K.Yanagi, T.Nishio, H.Hashimoto, M.Yoshizawa
    • Journal Title

      Chem.Phys.Lett. 408

      Pages: 89-95

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Time-resolved Absorption and Fluorescence Spectroscopy in Carotenoids Using Tunable Femtosecond Pump Pulses2005

    • Author(s)
      D.Kosumi, M.Komukai, K.Yanagi, H, Hashimoto, M.Yoshizawa
    • Journal Title

      Carotenoid Science 8(印刷中)

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Dynamics of Carotenoids Probed by Femtosecond Absorption, Fluorescence, and Raman Spectroscopy2005

    • Author(s)
      M.Yoshizawa, D.Kosumi, M.Komukai, K.Yanagi, H.Hashimoto
    • Journal Title

      Ultrafast Phenomena XIV, Springer Series in Chemical Physics (印刷中)

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Pump wavelength dependence of ultrafast relaxation kinetics in β-carotene2004

    • Author(s)
      D.Kosumi, H.Hashimoto, M.Yoshizawa
    • Journal Title

      Carotenoid Science 7

      Pages: 29-31

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Annual Research Report 2004 Final Research Report Summary
  • [Journal Article] The Very Early Events Following Photoexcitation of Carotenoids2004

    • Author(s)
      H.Hashimoto, K.Yanagi, M.Yoshizawa, D.Polli, G.Cerullo, G.Lanzani, S.De Silvestri, A.T.Gardiner, R.J.Cogdell
    • Journal Title

      Archives of Biochemistry and Biophysics 430

      Pages: 61-69

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] 誘導ラマン散乱による超高速時間分解振動分光2004

    • Author(s)
      吉澤雅幸
    • Journal Title

      分光研究 53

      Pages: 102-103

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] 光合成色素カロテノイドの超高速緩和過程2004

    • Author(s)
      橋本秀樹, 佐島徳武, 柳和宏, 吉澤雅幸
    • Journal Title

      レーザー研究 32

      Pages: 701-710

    • NAID

      10014032206

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Purple Bacterial Light-Harvesting Complexes : From Dreams to Structures2004

    • Author(s)
      R.J.Cogdell, H.Hashimoto, A.T.Gardiner
    • Journal Title

      Photosynth.Res. 80

      Pages: 173-179

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Protein Regulation of Carotenoid Binding : Gatekeeper and Locking Amino Acid Residues in Reaction Centers of Rhodobacter sphaeroides2004

    • Author(s)
      A.W.Roszak, K.McKendrick, A.T.Gardiner, I.A.Mitchell, N.W.Isaacs, R.J.Cogdell, H.Hashimoto, H.A.Frank
    • Journal Title

      Structure 12

      Pages: 765-773

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Stark spectroscopy on the LH2 complex from Rhodobacter sphaeroides G1C ; frequency and temperature dependence2004

    • Author(s)
      K.Yanagi, H.Hashimoto, A.T.Gardiner, R.J.Cogdell
    • Journal Title

      J.Phys.Chem.B 108

      Pages: 10334-10339

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Effect of the inhomogeneous band-broadening on the nonlinear optical properties of hydrazones2004

    • Author(s)
      K.Yanagi, A.T.Gardiner, R.J.Cogdell, H.Hashimoto
    • Journal Title

      J.Phys.B 69

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Ultrafast Time-Resolved Vibrational Spectroscopy Using Stimulated Raman Scattering (Japanese)2004

    • Author(s)
      M.Yoshizawa
    • Journal Title

      J.Spectro.Soc.Jpn. 53

      Pages: 102-103

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Ultrafast Relaxation Processes of Photosynthetic Carotenoids (Japanese)2004

    • Author(s)
      H.Hashimoto, T.Sashima, K.Yanagi, M.Yoshizawa
    • Journal Title

      Rev.Laser Engineer. 32

      Pages: 701-710

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Effect of the in homogeneous band-broadening on the nonlinear optical properties of hydrazones2004

    • Author(s)
      K.Yanagi, A.T.Gardiner, R.J.Cogdell, H.Hashimoto
    • Journal Title

      Phys.Rev.B 69

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] The Very Early Events Following Photoexcitation of Carotenoids2004

    • Author(s)
      H.Hashimoto, K.Yanagi, M.Yoshizawa, D.Polli, G.Cerullo, G.Lanzani, S.De Silvestri, A.T.Gardiner., R.J.Cogdell
    • Journal Title

      Archives of Biochemistry and Biophysics 430

      Pages: 61-69

    • Related Report
      2004 Annual Research Report
  • [Journal Article] 誘導ラマン散乱による超高速時間分解振動分光2004

    • Author(s)
      吉澤雅幸
    • Journal Title

      分光研究 53・2

      Pages: 102-103

    • Related Report
      2004 Annual Research Report
  • [Journal Article] 光合成色素カロテノイドの超高速緩和過程2004

    • Author(s)
      橋本秀樹, 佐島徳武, 柳和宏, 吉澤雅幸
    • Journal Title

      レーザー研究 32・11

      Pages: 701-710

    • NAID

      10014032206

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Ultrafast Relaxation Kinetics of Excited States in a Series of Mini- and Macro-β-Carotenes2003

    • Author(s)
      M.Yoshizawa, H.Aoki, M.Ue, H.Hashimoto
    • Journal Title

      Phys.Rev.B 67

    • NAID

      120000775829

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Ultrafast dynamics in a series of carotenoids investigated by time-resolved stimulated Raman spectroscopy2003

    • Author(s)
      M.Yoshizawa, H Hashimoto
    • Journal Title

      SPIE Proceedings of International Symposium on Optical Science and Technology 5212

      Pages: 13-22

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Ultrafast Relaxation Kinetics in Mini- and Macro-Carotenes Investigated by Femtosecond Absorption and Raman Spectroscopy2003

    • Author(s)
      M.Yoshizawa, H.Aoki, M.Ue, H.Hashimoto
    • Journal Title

      Carotenoid Science 6

      Pages: 24-25

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Origin of transition dipole-moment polarizability and hyperpolarizability in hydrazones2003

    • Author(s)
      K.Yanagi, T.Kobayashi, H.Hashimoto
    • Journal Title

      Phys.Rev.B 67

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Ultrafast Relaxation Kinetics of Excited States in a Series of Mini-and Macro-β-Carotenes2003

    • Author(s)
      M.Yoshizawa, H.Aoki, M.Ue, H.Hashimoto
    • Journal Title

      Phys.Rev.B 67

    • NAID

      120000775829

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Ultrafast dynamics in a series of carotenoids investigated by time-resolved stimulated Raman spectroscopy2003

    • Author(s)
      M.Yoshizawa, H.Hashimoto
    • Journal Title

      SPIE Proceedings of International Symposium on Optical Science and Technology 5212

      Pages: 13-22

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Ultrafast Relaxation Kinetics in Mini and Macro-Carotenes Investigated by Femtosecond Absorption and Raman Spectroscopy2003

    • Author(s)
      M.Yoshizawa, H.Aoki, M.Ue, H.Hashimoto
    • Journal Title

      Carotenoid Science 6

      Pages: 24-25

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Vibrational relaxation of excited states in a series of carotenes with several polyene lengths2002

    • Author(s)
      M.Yoshizawa, H.Hashimoto
    • Journal Title

      SPIE Proceedings of International Symposium on Optical Science and Technology 4812

      Pages: 15-23

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Molecular Structures of Carotenoids as Predicted by MNDO-AM1 Molecular Orbital Calculations2002

    • Author(s)
      H.Hashimoto, T.Yoda, T.Kobayashi, A.J.Young
    • Journal Title

      J.Mol.Struct. 604

      Pages: 125-146

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] The binding of xanthophylls to the bulk light-harvesting complex of photosystem II of higher plants : a specific requirement for carotenoids with a 3-hydrtoxy-β-end group2002

    • Author(s)
      D.Phillip, S.Hobe, H.Paulsen, P.Molnar, H.Hashimoto, A.J.Young
    • Journal Title

      J.Biol.Chem. 277

      Pages: 25160-25169

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Photosynthetic Light Harvesting by Carotenoids : Detection of an Intermediate Excited State2002

    • Author(s)
      G.Cerullo, D.Polli, G.Lanzani, S.DeSilvestri, H.Hashimoto, R.J.Cogdell
    • Journal Title

      Science 298

      Pages: 2395-2398

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Photosynthetic Light Harvesting by Carotenoids : Detection of an Intermediate Excited State2002

    • Author(s)
      G.Cerullo, D.Polli, G.Lanzani, S.De Silvestri, H.Hashimoto, R.J.Cogdell
    • Journal Title

      Science 298

      Pages: 2395-2398

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Publications] M.Yoshizawa, H.Aoki, M.Ue, H.Hashimoto: "Ultrafast Relaxation Kinetics of Excited States in a Series of Mini- and Macro-β-Carotenes"Phys.Rev.B. 67(17). 174302(1)-174302(8) (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] M.Yoshizawa, H.Aoki, M.Ue, H.Hashimoto: "Ultrafast Relaxation Kinetics in Mini-and Macro-Carotenes Investigated by Femtosecond Absorption and Raman Spectroscopy"Carotenoid Science. 6. 24-25 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] K.Yanagi, T.Kobayashi, H.Hashimoto: "Origin of transition dipole-moment polarizability and hyperpolarizability in hydrazones"Phys.Rev.B. 67(11). 115122(1)-115122(8) (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] A.Sugita, K.Yanagi, K.Kuroyanagi, H.Takahahsi, S.Aoshima, Y.Tsuchiya, S.Tasaka, H.Hashimoto: "Photo-excited state of N-benzyl MNA studied by femtosecond time-resolved absorption spectroscopy"Chem.Phys.Lett.. 382. 693-698 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] M.Yoshizawa, H.Hashimoto: "Ultrafast dynamics in a series of carotenoids investigated by time-resolved stimulated Raman"SPIE Proceedings of International Symposium on Optical Science and Technology. 5212. 13-22 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] A.W.Roszak, K.McKendrick, A.T.Gardiner, I.A.Mitchell, N.W.Isaacs, R.J.Cogdell, H.Hashimoto, H.A.Frank: "Protein regulation of carotenoid Binding : gatekeeper and locking amino acid residues in reaction centers of Rhodobacter sphaeroides"Structure. (印刷中). (2004)

    • Related Report
      2003 Annual Research Report
  • [Publications] M.Yoshizawa, H.Aoki, H.Hashimoto: "Femtosecond Time-Resolved Raman Signals on Ultrafast Dynamics in All-trans-β-Carotene"Bull. Chem. Soc. Jpn.. 75. 949-955 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] M.Yoshimoto: "Vibrational relaxation of excited states in a series of carotenes with several polyene lengths"SPIE Proceedings of International Symposium on Optical Science and Technology. 4812. 15-23 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] M.Yoshizawa, H.Aoki, M.Ue, H.Hashimoto: "Ultrafast Relaxation Kinetics in Mini-and Macro-Carotenes Investigated by Femtosecond Absorption and Raman Spectroscopy"Carotenoid Science. 6(印刷中). (2003)

    • Related Report
      2002 Annual Research Report
  • [Publications] H.Hashimoto, T.Yoda, T.Kobayashi, A.J.Young: "Molecular Structures of Carotenoids as Predicted by MNDO-AMl Molecular Orbital Calculations"J. Mol. Struct.. 604. 125-146 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] G.Cerullo, D.Polli, G.Lanzani, S.De Silvestri, H.Hashimoto, R.J.Cogdell: "Photosynthetic Light Harvesting by Carotenoids : Detection of an Intermediate Excited State"Science. 298. 2395-2398 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] D.Phillip, S.Hobe, H.Paulsen, P.Molnar, H.Hashimoto, A.J.Young: "The binding of xanthophylls to the bulk light-harvesting complex of photosystem II of higher plants : a specific requirement for carotenoids with a 3-hydrtoxy-β-end group"J. Biol. Chem.. 277. 25160-25169 (2002)

    • Related Report
      2002 Annual Research Report

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Published: 2002-04-01   Modified: 2020-05-15  

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