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Electron Spin-Selective spontaneous exciton dissociation in organic semiconductor solid-state films

Research Project

Project/Area Number 21H02015
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 35030:Organic functional materials-related
Research InstitutionKyushu University

Principal Investigator

Nakanotani Hajime  九州大学, 工学研究院, 准教授 (90633412)

Project Period (FY) 2021-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥17,680,000 (Direct Cost: ¥13,600,000、Indirect Cost: ¥4,080,000)
Fiscal Year 2023: ¥2,860,000 (Direct Cost: ¥2,200,000、Indirect Cost: ¥660,000)
Fiscal Year 2022: ¥2,470,000 (Direct Cost: ¥1,900,000、Indirect Cost: ¥570,000)
Fiscal Year 2021: ¥12,350,000 (Direct Cost: ¥9,500,000、Indirect Cost: ¥2,850,000)
Keywords自発配向分極 / 有機半導体 / 分子配向 / 巨大表面電位 / 励起子解離 / 電荷移動型励起状態 / 有機薄膜 / 三重項励起子 / 有機機能性材料 / 熱活性化遅延蛍光 / 三重項 / 励起スピン状態 / 励起子解離エネルギー / 励起子 / 電荷再結合
Outline of Research at the Start

有機分子系において、電子と正孔が弱く束縛された電荷移動型(CT)励起子のダイナミクスは、有機光半導体デバイスの動作原理の中核をなす物理現象である。特にCT励起子の解離過程は、光電変換素子においては電荷分離効率の向上に寄与するが、有機EL素子では発光効率の損失となる。そのため、励起子解離過程は極めて重要な物理過程といえる。しかし、CT励起子の解離過程における励起スピン状態の役割は、依然として未解明である。本研究では、CT励起子における励起スピン状態制御の基礎学理を基盤とし、励起子解離過程における励起スピン状態選択性を実証することで、“逆電子移動損失ゼロ”という革新的な光電変換素子を実現する。

Outline of Final Research Achievements

In this study, we focus on spontaneous exciton dissociation in polar organic semiconductor solid-state thin films and investigate the role of excited spin states in exciton dissociation events. We found that the exciton dissociation from the triplet excited state proceeds more favorably than that from the singlet excited state. Furthermore, minimizing the recombination probability between holes and electrons as much as possible found that the electron lifetime has an extremely long lifetime of over one month, even at room temperature, and that spatial information can also be retained. These experimental results revealed by this research not only provide design guidelines for opt-electric organic devices that realize highly efficient and ultra-long-lived charge-separated states but also lead to the creation of novel devices that control the physical phenomena of light absorb, charge accumulation, and light emission, thereby opening up further possibilities for organic electronics.

Academic Significance and Societal Importance of the Research Achievements

本研究では、励起子解離により生成した電荷(電子)は、有機薄膜中で1ヶ月間以上に渡って極めて安定に保持されているという事実を初めて見出した。またさらに、長時間保持されている電荷は、有機薄膜中で空間的にも保持されていることを実験的に確認した。これらの事実は、従来不安定であると考えられていた有機薄膜中の電荷(ラジカル状態)は、有機分子の極性によって誘起される自発配向分極の形成により、その有機薄膜界面で安定に保持可能であるということを意味し、光電変換素子の高性能化だけでなく撮像素子やメモリ素子など、将来のIOT社会構築に必須となる様々なデバイスに応用できる可能性があり、得られた学術的意義は大きい。

Report

(4 results)
  • 2023 Annual Research Report   Final Research Report ( PDF )
  • 2022 Annual Research Report
  • 2021 Annual Research Report
  • Research Products

    (22 results)

All 2024 2023 2022 2021 Other

All Journal Article (12 results) (of which Int'l Joint Research: 5 results,  Peer Reviewed: 12 results,  Open Access: 1 results) Presentation (9 results) (of which Int'l Joint Research: 1 results,  Invited: 3 results) Remarks (1 results)

  • [Journal Article] Enhancing Triplet?Triplet Upconversion Efficiency and Operational Lifetime in Blue Organic Light-Emitting Diodes by Utilizing Thermally Activated Delayed Fluorescence Materials2023

    • Author(s)
      Nguyen Thanh B.、Nakanotani Hajime、Chan Chin-Yiu、Kakumachi Shunta、Adachi Chihaya
    • Journal Title

      ACS Applied Materials & Interfaces

      Volume: 15 Issue: 19 Pages: 23557-23563

    • DOI

      10.1021/acsami.3c02855

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Abrupt exciton quenching in blue fluorescent organic light-emitting diodes around turn-on voltage region2023

    • Author(s)
      Shunta Kakumachi, Thanh Ba Nguyen, Hajime Nakanotani, Chihaya Adachi
    • Journal Title

      Chemical Engineering Journal

      Volume: 471 Pages: 144516-144516

    • DOI

      10.1016/j.cej.2023.144516

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] A polar transition of spontaneous orientation polarization in organic amorphous thin films2023

    • Author(s)
      Yuuhi Ueda, Masaki Tanaka, Hajime Nakanotani, Chihaya Adachi
    • Journal Title

      Chemical Physics Letters

      Volume: 833 Pages: 140915-140915

    • DOI

      10.1016/j.cplett.2023.140915

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] The role of spontaneous orientation polarization on charge storage behavior at an interface between organic semiconductor layers2023

    • Author(s)
      Takahiko Yamanaka, Hajime Nakanotani, Chihaya Adachi
    • Journal Title

      Journal of Materials Chemistry C

      Volume: 12 Issue: 3 Pages: 1055-1060

    • DOI

      10.1039/d3tc03979j

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Anti-Stokes Luminescence in Multi-Resonance-Type Thermally-Activated Delayed Fluorescence Molecules2023

    • Author(s)
      Shintaro Kohata, Hajime Nakanotani, Youhei Chitose, Takuma Yasuda, Youichi Tsuchiya, Chihaya Adachi
    • Journal Title

      Angewandte Chemie International Edition

      Volume: 62 Issue: 44

    • DOI

      10.1002/anie.202312326

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Electron Lifetime of Over One Month in Disordered Organic Solid‐State Films2023

    • Author(s)
      Yamanaka Takahiko、Nakanotani Hajime、Nakamoto Katsuhiro、Adachi Chihaya
    • Journal Title

      Advanced Materials

      Volume: 35 Issue: 11 Pages: 2210335-2210338

    • DOI

      10.1002/adma.202210335

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] An Overlooked Charge‐Transfer Interaction in the Interfacial Triplet?Triplet Upconversion Process in Blue Organic Light‐Emitting Diodes2022

    • Author(s)
      Nguyen Thanh Ba、Nakanotani Hajime、Adachi Chihaya
    • Journal Title

      Advanced Optical Materials

      Volume: 10 Issue: 18 Pages: 2200704-2200704

    • DOI

      10.1002/adom.202200704

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Modulation of Intersystem Crossing Rate Induced by Singlet-triplet Energy Level Alignment in 1,2,3,5-Tetrakis(carbazol-9-yl)-4,6-dicyanobenzene Single Crystals2022

    • Author(s)
      Kohata Shintaro、Nakanotani Hajime、Adachi Chihaya
    • Journal Title

      Chemistry Letters

      Volume: 51 Issue: 10 Pages: 989-992

    • DOI

      10.1246/cl.220304

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Significant role of spin-triplet state for exciton dissociation in organic solids2022

    • Author(s)
      Yamanaka Takahiko、Nakanotani Hajime、Adachi Chihaya
    • Journal Title

      Science Advances

      Volume: 8 Issue: 9

    • DOI

      10.1126/sciadv.abj9188

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Direct Observation of Photoexcited Electron Dynamics in Organic Solids Exhibiting Thermally Activated Delayed Fluorescence via Time‐Resolved Photoelectron Emission Microscopy2021

    • Author(s)
      Fukami Yusuke、Iwasawa Masato、Sasaki Masahiro、Hosokai Takuya、Nakanotani Hajime、Adachi Chihaya、Fukumoto Keiki、Yamada Yoichi
    • Journal Title

      Advanced Optical Materials

      Volume: 9 Issue: 19 Pages: 2100619-2100619

    • DOI

      10.1002/adom.202100619

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Tetrabenzo[a,c]phenazine Backbone for Highly Efficient Orange-Red Thermally Activated Delayed Fluorescence with Completely Horizontal Molecular Orientation2021

    • Author(s)
      Balijapalli Umamahesh、Lee Yi‐Ting、Karunathilaka Buddhika S. B.、Tumen‐Ulzii Ganbaatar、Auffray Morgan、Tsuchiya Youichi、Nakanotani Hajime、Adachi Chihaya
    • Journal Title

      Angewandte Chemie International Edition

      Volume: 60 Issue: 35 Pages: 19364-19373

    • DOI

      10.1002/anie.202106570

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 2,6‐Dicarbonitrile Diphenyl‐1λ5 ‐Phosphinine (DCNP) A Robust Conjugated Building Block for Multi‐Functional Dyes Exhibiting Tunable Amplified Spontaneous Emission2021

    • Author(s)
      Balijapalli Umamahesh、Tang Xun、Okada Daichi、Lee Yi‐Ting、Karunathilaka Buddhika S. B.、Auffray Morgan、Tumen‐Ulzii Ganbaatar、Tsuchiya Youichi、Sandanayaka Atula S. D.、Matsushima Toshinori、Nakanotani Hajime、Adachi Chihaya
    • Journal Title

      Advanced Optical Materials

      Volume: 9 Issue: 21 Pages: 2101122-2101122

    • DOI

      10.1002/adom.202101122

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Presentation] 熱活性化遅延蛍光分子の進展:有機EL からフォトンアップコンバージョン2024

    • Author(s)
      中野谷 一
    • Organizer
      日本化学会第104回春季年会
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] 熱活性化遅延蛍光分子におけるアンチストークス発光2024

    • Author(s)
      木幡真太郎, 中野谷一, 安達千波矢
    • Organizer
      第71回応用物理学会春季学術講演会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Enhancing TTU-OLED performances by utilizing TADF Materials2023

    • Author(s)
      Thanh Ba Nguyen, Hajime Nakanotani, Chin-Yiu Chan, Shunta Kakumachi, Chihaya Adachi
    • Organizer
      有機EL討論会第36回例会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Research on Anti-Stokes Luminescence in Thermally Activated Delayed Fluorescence Molecules2023

    • Author(s)
      木幡真太郎, 中野谷一, 安達千波矢
    • Organizer
      2023年光化学討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] 青色蛍光OLEDの駆動電圧付近で生じる急激な励起消滅過程2023

    • Author(s)
      角町 駿太, Thanh Ba Nguyen, 中野谷 一, 安達 千波矢
    • Organizer
      第84回 応用物理学会 秋季学術講演会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Abrupt exciton quenching in blue fluorescent organic light-emitting diodes around turn-on voltage region2023

    • Author(s)
      角町 駿太, Thanh Ba Nguyen, 中野谷 一, 安達 千波矢
    • Organizer
      The 15th Asian Conference on Organic Electronics
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 青色蛍光OLEDの駆動電圧付近で生じる急激な励起子消滅過程2023

    • Author(s)
      角町 駿太, Thanh Ba Nguyen, 中野谷 一, 安達 千波矢
    • Organizer
      有機EL討論会 第37回例会
    • Related Report
      2023 Annual Research Report
  • [Presentation] 有機薄膜中での自発的な励起子解離現象とその応用2022

    • Author(s)
      中野谷 一
    • Organizer
      第71回高分子討論会
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Spontaneous dissociation of charge-transfer type excitons in organic solid-state films2022

    • Author(s)
      Hajime Nakanotani
    • Organizer
      日本化学会第102春季年会
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Remarks] 次世代有機LED材料の電子の動きを直接観察することに成功

    • URL

      https://www.kyushu-u.ac.jp/ja/researches/view/621

    • Related Report
      2021 Annual Research Report

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Published: 2021-04-28   Modified: 2025-01-30  

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