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Nonlinear interaction of excitons and photoinduced phase transition in quasi-one dimensional organic charge-transfer crystals

Research Project

Project/Area Number 11215204
Research Category

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

Allocation TypeSingle-year Grants
Review Section Science and Engineering
Research InstitutionOsaka University (2001)
Nagoya University (1999-2000)

Principal Investigator

TANIMURA Katsumi  The Institute of Scientific and Industrial Research, Osaka Univ., Professor, 産業科学研究所, 教授 (00135328)

Co-Investigator(Kenkyū-buntansha) ITOH Chihiro  Faculty of System Engineering, Wakayama Univ., Associate Professor, システム工学部, 助教授 (60211744)
AKIMOTO Ikuko  Faculty of System Engineering, Wakayama Univ., Research Associate (00314055)
Project Period (FY) 1999 – 2001
Project Status Completed (Fiscal Year 2001)
Budget Amount *help
¥55,500,000 (Direct Cost: ¥55,500,000)
Fiscal Year 2001: ¥6,800,000 (Direct Cost: ¥6,800,000)
Fiscal Year 2000: ¥44,200,000 (Direct Cost: ¥44,200,000)
Fiscal Year 1999: ¥4,500,000 (Direct Cost: ¥4,500,000)
KeywordsPhotoinduced phase transition / Charge-transfer crystals / Femtosecond spectroscopy / Initial-condition sensitivity / Proliferation / Nonlinear relaxation / 電荷移動有機錯体 / 光誘起構造相転位 / TTF-CA / 非線形相互作用
Research Abstract

The purpose of this project is to clarify the dynamics of photoinduced ionic-to-neutral phase transition (NI transition) in one-dimensional organic charge-transfer crystal of tetrathiafulvalen-p-chloranil (TTF-CA) for understanding the mechanism of this photoinduced process from microscopic point of view. We have studied the temporal evolution of the process by means of time-resolved reflectance spectroscopy in temporal domains of sub-ps, and the state-sensitive efficiency of the phase transition by means of excitation spectroscopy, using a tunable ns laser from 266 to 2000 nm. Main results obtained are summarized below.
1) The whole process of the photoinduced NI transition in TTF-CA consists of the three sequential primary steps ; the first is the precursor-forming process at a few ps after excitation, the second is the process of local proliferation around 50 ps after excitation, and the third is the process of forming N-phase orders, lasting over 300 ps.
2) The process of precursor formation is nonlinear in the sense that one-absorbed photon converts the charge state of as many as a few hundreds of donor-acceptor molecules to form individual neutral-molecular clusters on stack chains. The proliferation in this process is strongly excitation-wavelength dependent, showing the initial-condition sensitivity in this photoinduced transformation.
3) The second and third processes are associated with nonlinear proliferation of photoinduced changes ; the magnitudes of proliferation depend strongly on the amount of the precursor photoinduced. This proliferation of nonlinear relaxation also dependents on temperature, and the magnitude is governed by an activation energy of 0.01eV, which roughly corresponds to the free-energy difference between the two phases.
These results have provided us crucial knowledge for establishing thorough understanding of the mechanism of this photoinduced phase transition.

Report

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

    (35 results)

All Other

All Publications (35 results)

  • [Publications] T.Suzuki, T.Sakamaki, K.Tanimura, S.Koshihara, Y.Tokura: "Ionic-to-neutral phase transformation induced by photoexcitation of the charge-transfer band in tetrathiafulvalen-p-chloranil crystals"Phys.Rev.B. 60. 6191-6193 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] C.Itoh, T.Kondoh, K.Tanimura: "Photo-induced dimer-diradical formation in diacetylene crystals at low temperatures"J.Phys.Soc.Jpn.. 68. 1711-1715 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] A.L.Shluger, K.Tanimura: "Laser-induced reactions in crystals:Femtosecond pump-probe spectroscopy and ab-initio calculations of self-trapped excitons and holes in KBr"Phys.Rev.B. 61. 5392-5402 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K.Tanimura, S.Koshihara: "Photo-induced Ionic-to-Neutral phase transition in tetrathiafulvalen-p-chloranil crystals"Phase Transitions. 74. 21-34 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T.Kondoh, C.Itoh, K.Tanimura: "Selective polymerization of 5,7-dodecadiyne-1,12-diol bis[phenylcarbamate](TCDU)crystals and thermochromism of the polymerized crystals"J.Phys.Soc.Jpn.. 70. 1817 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K.Tanimura: "Femtosecond time-resolved spectroscopy of formation of self-trapped excitons in CaF_2"Phys.Rev.B. 63. 184303 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K.Tanimura, I.Akimoto: "Femtosecond time-resolved spectroscopy of photoinduced ionic-to-neutral phase transition in tetrathiafulvalen-p-chloranil crystals"J.Lumin. 94-95. 483 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] I.Akimoto, K.Tanimura, S.Koshihara: "Dynamics of the photoinduced ionic-to-neutral phase transition in tetrathiafulvalene-p-chloranil studied by femtosecond time-resolved reflection spectroscopy"Phase Transitions. (in print).

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K.Tanimura, I.Akimoto: "Initial-condition sensitivity and nonlinear relaxation in photo-induced ionic-to-neutral phase transition in tetrathiafulvalen-p-chloranil crystals"Phase Transitions. (in print).

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] C.Itoh, M.Shirai, K.Tanaka, K.Kan'no: "Pulsed-ESR study of spin solitons as a probe of neutral-to-ionic phase transition of TTF-CA single crystal"Phase Transitions. (in print).

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] C.Itoh, T.Kondoh, K.Tanimura: "Exciton self-trapping and formation of dimer diradicals in 5,7-dodecadiyne-1,12-diol bis[phenylcarbamate](TCDU)at low temperatures"Phys.Rev.B. (in print).

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T. Suzuki, T. Sakamaki, K. Tanimura, S. Koshihara, and Y. Tokura: "Ionic-to-neutral phase transformation induced by photoexcitation of the charge-transfer band in tetrathiafulvalen-p-chloranil crystals"Phys. Rev. B. 60. 6191-6193 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] C. Itoh, T. Kondoh, and K. Tanimura: "Photo-induced dimer-diradical formation in diacetylene crystals at low temperatures"J. Phys. Soc. Jpn.. 68. 1711-1715 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] A. L. Shluger and K. Tanimura: "Laser-induced reactions in crystals : Femtosecond pump-probe spectroscopy and ab-initio calculations of self-trapped excitons and holes in KBr"Phys. Rev. B. 61. 5392-5402 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K. Tanimura and S. Koshihara: "Photo-induced Ionic-to-Neutral phase transition in tetrathiafulvalen-p-chloranil crystals"Phase Transitions. 74. 21-34 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T. Kondoh, C. Itoh, and K. Tanimura: "Selective polymerization of 5,7-dodecadiyne-1,12-diol bis[phenylcarbamate](TCDU) crystals and thermochromism of the polymerized crystals"J. Phys. Soc. Jpn.. 70. 1817-1824 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K. Tanimura: "Femtosecond time-resolved spectroscopy of formation of self-trapped excitons in CaF_2"Phys. Rev. B. 63. 184303-1-4 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K. Tanimura and I. Akimoto: "Femtosecond time-resolved spectroscopy of photoinduced ionic-to-neutral phase transition in tetrathiafulvalen-p-chloranil crystals"J. Lumin. 94-95. 483-488 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] I. Akimoto, K. Tanimura, and S. Koshihara: "Dynamics of the photoinduced ionic-to-neutral phase transition in tetrathiafulvalene-p-chloranil studied by femtosecond time-resolved reflection spectroscopy"Phase Transitions. (in print).

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K. Tanimura and I. Akimoto: "Initial-condition sensitivity and nonlinear relaxation in photo-induced ionic-to-neutral phase transition in tetrathiafulvalen-p-chloranil crystals"Phase Transitions. (in print).

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] C. Itoh, M. Shirai, K. Tanaka and K. Kan'no: "Pulsed-ESR study of spin solitons as a probe of neutral-to-ionic phase transition of TTF-CA single crystal"Phase Transitions. (in print).

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] C. Itoh, T. Kondoh, and K. Tanimura: "Exciton self-trapping and formation of dimer diradicals in 5,7-dodecadiyne-1,12-diol bis[phenylcarbamate](TCDU) at low temperatures"Phys. Rev. B. (in print).

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T.Suzuki, T.Sakamaki, K.Tanimura, S.Koshihara, Y.Tokura: "Ionic-to-neutral phase transformation induced by photoexcitation of the charge-transfer band in tetrathiafulvalen-p-chloranil crystals"Phys.Rev.B. 60. 6191-6193 (1999)

    • Related Report
      2001 Annual Research Report
  • [Publications] C.Itoh, T.Kondoh, K.Tanimura: "Photo-induced dimer-diradical formation in diacetylene crystals at low temperatures"J.Phys.Soc.Jpn.. 68. 1711-1715 (1999)

    • Related Report
      2001 Annual Research Report
  • [Publications] A.L.Shluger, K.Tanimura: "Laser-induced reactions in crystals : Femtosecond pump-probe spectroscopy and ab-initio calculations of self-trapped excitons and holes in KBr"Phys.Rev.B. 61. 5392-5402 (2000)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Tanimura, S.Koshihara: "Photo-induced Ionic-to-Neutral phase transition in tetrathiafulvalen-p-chloranil crystals"Phase Transitions. 74. 21-34 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] T.Kondoh, C.Itoh, K.Tanimura: "Selective polymerization of 5,7-dodecadiyne-1,12-diol bis[phenylcarbamate](TCDU) crystals and thermochromism of the polymerized crystals"J.Phys.Soc.Jpn.. 70. 1817 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Tanimura: "Femtosecond time-resolved spectroscopy of formation of self-trapped excitons in CaF_2"Phys.Rev.B. 63. 184303 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Tanimura, I.Akimoto: "Femtosecond time-resolved spectroscopy of photoinduced ionic-to-neutral phase transition in tetrathiafulvalen-p-chloranil crystals"J.Lumin. 94-95. 483 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] I.Akimoto, K.Tanimura, S.Koshihara: "Dynamics of the photoinduced ionic-to-neutral phase transition in tetrathiafulvalene-p-chloranil studied by femtosecond time-resolved reflection spectroscopy"Phase Transitions. (in print).

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Tanimura, I.Akimoto: "Initial-condition sensitivity and nonlinear relaxation in photo-induced ionic-to-neutral phase transition in tetrathiafulvalen-p-chloranil crystals"Phase Transitions. (in print).

    • Related Report
      2001 Annual Research Report
  • [Publications] C.Itoh, M.Shirai, K.Tanaka, K.Kanno: "Pulsed-ESR study of spin solitons as a probe of neutral-to-ionic phase transition of TTF-CA single crystal"Phase Transitions. (in print).

    • Related Report
      2001 Annual Research Report
  • [Publications] C.Itoh, T.Kondoh, K.Tanimura: "Exciton self-trapping and formation of dimer diradicals in5,7-dodecadiyne-1,12-diol bis[phenylcarbamate](TCDU) at low temperatures"Phys.Rev.B. (in print).

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Tanimura and S.Koshihara: "Photo-induced ionic-to-neutral phasetransition in tetrathiafulvalen-p-chloranil crystals"Phase Transition. Special Volume(in print). (2001)

    • Related Report
      2000 Annual Research Report
  • [Publications] T.Kondoh,C.Itoh,and K.Tanimura: "Selective polymerization of 5,7-dodecadiyne-1,12-diol bis (phenylcarbamate) crystals and thermochromism of polymers"J.Phys.Soc.Jpn.. (in print). (2001)

    • Related Report
      2000 Annual Research Report

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

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