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有機-無機複合分子協調による励起子ダイナミクスの精密制御と機能発現

Publicly Offered Research

Project AreaApplication of Cooperative-Excitation into Innovative Molecular Systems with High-Order Photo-functions
Project/Area Number 17H05270
Research Category

Grant-in-Aid for Scientific Research on Innovative Areas (Research in a proposed research area)

Allocation TypeSingle-year Grants
Review Section Science and Engineering
Research InstitutionKeio University

Principal Investigator

羽會部 卓  慶應義塾大学, 理工学部(矢上), 准教授 (70418698)

Project Period (FY) 2017-04-01 – 2019-03-31
Project Status Completed (Fiscal Year 2018)
Budget Amount *help
¥7,930,000 (Direct Cost: ¥6,100,000、Indirect Cost: ¥1,830,000)
Fiscal Year 2018: ¥4,030,000 (Direct Cost: ¥3,100,000、Indirect Cost: ¥930,000)
Fiscal Year 2017: ¥3,900,000 (Direct Cost: ¥3,000,000、Indirect Cost: ¥900,000)
Keywords有機・無機複合材料 / 有機ー無機複合材料 / 励起ダイナミクス制御 / 有機無機複合材料 / 有機無機複合体 / 励起状態制御
Outline of Annual Research Achievements

有機薄膜や分子集合体内での励起子とキャリア電荷に関する生成・移動の制御はエレクトロニクス・光エネルギー変換分野で非常に重要な課題である。本研究では分子集合体における一重項分裂(Singlet Fission: SF)の発現と逐次反応への展開をめざし、ペンタセンやテトラセン等のアセン系分子を用いた二量体や有機-無機複合材料の合成と物性評価に取り組んだ。まず、フェニルおよびビフェニルをリンカーとする各種のペンタセン二量体では、色素間の相互作用の段階的な制御に伴う量論的SFと励起三重項状態の長寿命化に成功した。特に、時間分解ESR測定では、相関のある三重項対(TT)に対応する五重項状態が独立した三重項対(T + T)の生成に関与することを速度論的に明らかにした。環状三量体のペンタセンナノチューブでは、環状構造として初のSF観測に成功した。
次に、有機無機複合体への展開として、ペンタセン修飾アルカンチオール単分子膜 (SAMs)で保護された金ナノクラスターではペンタセンの励起一重項状態から金表面への迅速なエネルギー移動を抑え、ΦT = 172%の三重項量子収率で金属表面上でのSFの観測は既に報告している。この結果を踏まえて、ペンタセンとペリレンジイミド (PDI)の混合SAMsでは単分子膜であるため2つの色素の被覆率を系統的に変化させることができ、色素濃度比に依存した励起ダイナミクス制御(SF、電子移動およびエキシマー)を明らかにした。

Research Progress Status

平成30年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

平成30年度が最終年度であるため、記入しない。

Report

(2 results)
  • 2018 Annual Research Report
  • 2017 Annual Research Report
  • Research Products

    (18 results)

All 2019 2018 2017 Other

All Int'l Joint Research (2 results) Journal Article (7 results) (of which Int'l Joint Research: 7 results,  Peer Reviewed: 7 results) Presentation (9 results) (of which Int'l Joint Research: 3 results,  Invited: 5 results)

  • [Int'l Joint Research] タンペレ工科大(フィンランド)

    • Related Report
      2018 Annual Research Report
  • [Int'l Joint Research] Tampere University of Technology(フィンランド)

    • Related Report
      2017 Annual Research Report
  • [Journal Article] Quantitative Sequential Photoenergy Conversion Process from Singlet Fission to Intermolecular Two-Electron Transfers Utilizing Tetracene Dimer2018

    • Author(s)
      Nakamura Shunta、Sakai Hayato、Nagashima Hiroki、Kobori Yasuhiro、Tkachenko Nikolai V.、Hasobe Taku
    • Journal Title

      ACS Energy Letters

      Volume: 4 Issue: 1 Pages: 26-31

    • DOI

      10.1021/acsenergylett.8b01964

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] A Pentacene-based Nanotube Displaying Enriched Electrochemical and Photochemical Activities2018

    • Author(s)
      Kuroda Kiyonori、Yazaki Kohei、Tanaka Yuya、Akita Munetaka、Sakai Hayato、Hasobe Taku、Tkachenko Nikolai V.、Yoshizawa Michito
    • Journal Title

      Angewandte Chemie International Edition

      Volume: 58 Issue: 4 Pages: 1115-1119

    • DOI

      10.1002/anie.201812976

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] High‐Yield Generation of Triplet Excited States by an Efficient Sequential Photoinduced Process from Energy Transfer to Singlet Fission in Pentacene‐Modified CdSe/ZnS Quantum Dots2018

    • Author(s)
      Sakai Hayato、Inaya Ryutaro、Tkachenko Nikolai V.、Hasobe Taku
    • Journal Title

      Chemistry - A European Journal

      Volume: 24 Issue: 64 Pages: 17062-17071

    • DOI

      10.1002/chem.201803257

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Multiexciton Dynamics Depending on Intramolecular Orientations in Pentacene Dimers: Recombination and Dissociation of Correlated Triplet Pairs2018

    • Author(s)
      Sakai Hayato、Inaya Ryutaro、Nagashima Hiroki、Nakamura Shunta、Kobori Yasuhiro、Tkachenko Nikolai V.、Hasobe Taku
    • Journal Title

      The Journal of Physical Chemistry Letters

      Volume: 9 Issue: 12 Pages: 3354-3360

    • DOI

      10.1021/acs.jpclett.8b01184

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Concentration-dependent photophysical switching in mixed self-assembled monolayers of pentacene and perylenediimide on gold nanoclusters2018

    • Author(s)
      D. Kato, H. Sakai, Y. Araki, T. Wada, N. V. Tkachenko, T. Hasobe
    • Journal Title

      Phys. Chem. Chem. Phys.

      Volume: 20 Issue: 13 Pages: 8695-8706

    • DOI

      10.1039/c8cp00174j

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Synthesis, Structural and Photophysical Properties of Pentacene Alkanethiolate Monolayer-Protected Gold Nanoclusters and Nanorods: Supramolecular Intercalation and Photoinduced Electron Transfer with C602017

    • Author(s)
      Kato Daiki、Sakai Hayato、Saegusa Toshiyuki、Tkachenko Nokolai V.、Hasobe Taku
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 121 Issue: 16 Pages: 9043-9052

    • DOI

      10.1021/acs.jpcc.7b01164

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Inter- and Intramolecular Electron-Transfer Reduction Properties of Coronenediimide Derivatives via Photoinduced Processes2017

    • Author(s)
      Yoshida Motoki、Sakai Hayato、Ohkubo Kei、Fukuzumi Shunichi、Hasobe Taku
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 122 Issue: 25 Pages: 13333-13346

    • DOI

      10.1021/acs.jpcc.7b09817

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Presentation] High-yield singlet fission and sequential photoinduced process in acene-based molecular assemblies2019

    • Author(s)
      Taku Hasobe
    • Organizer
      International Workshop Photofunctional Materials Using Spin Degrees of Freedom: Interplay among synthesis, measurement, and theory.
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Structural and Photophysical Properties of Pentacene-based Self-assembled Monolayers on Gold Nanomaterials2018

    • Author(s)
      T. Hasobe and Hayato Sakai
    • Organizer
      233rd The Electrochemical Society Center Meeting
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 光機能発現に向けた有機材料の設計戦略と応用展開2018

    • Author(s)
      羽曾部 卓
    • Organizer
      電気化学会関東支部主催 第54回学際領域セミナー「光電気化学的応用のためのナノマテリアル設計」
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] 二次元π共役分子および集合体の励起ダイナミクス制御2018

    • Author(s)
      羽曾部 卓
    • Organizer
      日本化学会低次元系光機能材料研究会 第7回研究講演会―二次元構造を有するπ電子系の光・電子機能―
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] 新規ヘキサセン二量体の合成と高効率な一重項分裂の発現2018

    • Author(s)
      中村 俊太・酒井 隼人・ Nikolai V. Tkachenko・羽曾部 卓
    • Organizer
      第29回基礎有機化学討論会
    • Related Report
      2018 Annual Research Report
  • [Presentation] ペンタセンダイマー修飾CdSe/ZnSナノ粒子におけるエネルギー移動と一重項分裂の逐次的反応進行2018

    • Author(s)
      稲谷 隆太郎・酒井 隼人・TKACHENKO Nikolai・羽曾部 卓
    • Organizer
      日本化学会 第98春季年会
    • Related Report
      2017 Annual Research Report
  • [Presentation] テトラセンアルカンチオール修飾金ナノクラスターの構造制御と一重項分裂を介した長寿命三重項励起子の生成2018

    • Author(s)
      三枝 稔幸・酒井 隼人・TKACHENKO Nikolai・羽曾部 卓
    • Organizer
      日本化学会 第98春季年会
    • Related Report
      2017 Annual Research Report
  • [Presentation] High-Yield and Long-Lived Triplet Excited States of Pentacene Alkanethiolate Monolayer Protected Gold Nanoparticles by Singlet Fission2017

    • Author(s)
      Taku Hasobe and Hayato Sakai
    • Organizer
      231th The Electrochemical Society Center Meeting
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] テトラセンアルカンチオール修飾金ナノ粒子の色素間配向制御による長寿命励起三重項状態の生成2017

    • Author(s)
      三枝 稔幸・酒井 隼人・Tkachenko Nikolai・羽曾部 卓
    • Organizer
      2017年光化学討論会
    • Related Report
      2017 Annual Research Report

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Published: 2017-04-28   Modified: 2019-12-27  

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