Organic Thin-Film Superconductor Based on Electric Polarization

• Project/Area Number: 21K18210
• Research Category: Grant-in-Aid for Challenging Research (Pioneering)
• Allocation Type: Multi-year Fund
• Review Section: Medium-sized Section 35:Polymers, organic materials, and related fields
• Research Institution: Kyushu University
• Principal Investigator: 安達 千波矢 九州大学, 工学研究院, 教授 (30283245)
• Co-Investigator(Kenkyū-buntansha): 松島 敏則 九州大学, カーボンニュートラル・エネルギー国際研究所, 准教授 (40521985) ; 合志 憲一 九州大学, 工学研究院, 助教 (50462875) ; 中野谷 一 九州大学, 工学研究院, 准教授 (90633412)
• Project Period (FY): 2021-07-09 – 2023-03-31
• Project Status: Discontinued (Fiscal Year 2022)
• Budget Amount: ¥26,000,000 (Direct Cost: ¥20,000,000、Indirect Cost: ¥6,000,000); Fiscal Year 2023: ¥8,840,000 (Direct Cost: ¥6,800,000、Indirect Cost: ¥2,040,000); Fiscal Year 2022: ¥8,840,000 (Direct Cost: ¥6,800,000、Indirect Cost: ¥2,040,000); Fiscal Year 2021: ¥8,320,000 (Direct Cost: ¥6,400,000、Indirect Cost: ¥1,920,000)
• Keywords: 有機超伝導体 / 有機CT / 電子分極 / ペロブスカイト構造 / 有機・無機ハイブリッド / Little/Ginzburg / 有機超伝導 / CT錯体 / Ginzburg / Little / 二次元ペロブスカイト / F16CuPc / mMTDATA / 有機積層薄膜 / GSP

Outline of Research at the Start

電子分極誘電層(P)/導電層(C)/電子分極誘電層(P)の3層を基本構造とし、薄膜導電層中の伝導電子と誘電層内の分極性分子との間で電子分極効果に基づく“クーパー対”形成を目指す。電子分極誘電層には、様々なドナー及びアクセプター分子骨格を含有したπ電子系化合物を用いることでCT強度を精密に調整し、電子分極により伝導層内のクーパー電子対形成を目指す。基礎的な材料設計及びデバイス構造設計を確立し、①電子分極強度とクーパー対形成の相関、②超伝導転移温度（Tc）向上の可能性を探る。電子分極構造と導電層の網羅的な材料検討・最適化によるTc向上について研究を進め、室温有機超伝導体の可能性に繋げる。

Outline of Annual Research Achievements

本研究では、Little/Ginzburgのモデルを基礎に、近年、有機光エレクトロニクス研究分野で培われてきた新規な有機系CT材料や薄膜中で特異的に大きな分極（GSP: Giant Spontaneous Polarization）を示す分子系材料、さらには、近年、太陽電池等で大きな注目を集めている有機無機ハイブリッドペロブスカイト化合物を利用し、積層薄膜型室温有機超伝導の実現を目指している。具体的には、それらの構造中に、電子分極誘電層/導電層/電子分極誘電層を導入し、薄膜導電層中の伝導電子と誘電層内の分極性分子との間で電子分極効果を発現することでクーパー対の形成を目指している。本研究では、これらの電子分極機構を構築できる系として有機・無機2次元ペロブスカイト系に着目し、電子分極性の大きいNDIを組み込んだ2次元ペロブスカイト構造を構築した（Adv. Opt. Mat.）。本系においては、タイプII型のヘテロ構造を構成することを明らかにした。理論計算及び実験結果から、有機配位子と無機層の間で電荷移動が生じることを時間分解発光スペクトルの解析及び光電変換特性から明らかにし、両層間における電荷移動の存在を明らかにした。今後、様々な有機層の検討により、電子分極の可能性を追究していく。一方で、薄膜金属を有機層で積層したGinzburgのモデルにおいても、Mg合金を用いることで5nmの均一な超薄膜金属層を有機薄膜上に形成できることを確立した。今後、両素子において、低温物性の検討を進め、有機配位子及び有機層の電子分極効果を確認していく予定である。

Research Products

• [Int'l Joint Research] ソルボンヌ大学/CNRS（フランス国立科学研究センター）(フランス)
• [Int'l Joint Research] Sorbonne University-CNRS(フランス)
• [Journal Article] Artificial p-n‐like Junction Based on Pure 2D Organic-Inorganic Halide Perovskite Structure Having Naphthalene Diimide Acceptor Moieties (2023)
  • Author(s): Zhao Feng, Xuelong Liu, Kentaro Imaoka, Tomohiro Ishii, Ganbaatar Tumen‐Ulzii, Xun Tang, George F Harrington, Benoit Heinrich, Jean‐Charles Ribierre, Lise‐Marie Chamoreau, Lydia Sosa Vargas, David Kreher, Kenichi Goushi, Toshinori Matsushima, Guijiang Zhou, Fabrice Mathevet, Chihaya Adachi
  • Journal Title: Advanced Optical Materials Volume: 2202734 Issue: 10 Pages: 1-8
  • DOI: 10.1002/adom.202202734
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Advanced Organic Laser System Having Triplet Scavengers (2021)
  • Author(s): Buddhika S. B. Karunathilaka, Umamahesh Balijapalli, Toshinori Matsushima*, Atula S. D. Sandanayaka*, and Chihaya Adachi*
  • Journal Title: NIHON GAZO GAKKAISHI (Journal of the Imaging Society of Japan) Volume: 60 Issue: 6 Pages: 615-630
  • DOI: 10.11370/isj.60.615
  • NAID: 130008128289
  • ISSN: 1344-4425, 1880-4675
  • Year and Date: 2021-12-10
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Organic long-persistent luminescence stimulated by visible light in p-type systems based on organic photoredox catalyst dopants (2021)
  • Author(s): Jinnai Kazuya、Kabe Ryota、Lin Zesen、Adachi Chihaya
  • Journal Title: Nature Materials Volume: 21 Issue: 3 Pages: 338-344
  • DOI: 10.1038/s41563-021-01150-9
  • Peer Reviewed
• [Journal Article] Visualization of Frontier Molecular Orbital Separation of a Single Thermally Activated Delayed Fluorescence Emitter by STM (2021)
  • Author(s): Zoh Inhae、Imai-Imada Miyabi、Bae Jaehyun、Imada Hiroshi、Tsuchiya Youichi、Adachi Chihaya、Kim Yousoo
  • Journal Title: The Journal of Physical Chemistry Letters Volume: 12 Issue: 31 Pages: 7512-7518
  • DOI: 10.1021/acs.jpclett.1c02140
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Low-threshold exciton-polariton condensation via fast polariton relaxation in an organic microcavities (2021)
  • Author(s): T. Ishii, K. Miyata, M. Mamada, F. Bencheikh, F. Mathevet, K. Onda, S. Kena-Cohen, C. Adachi
  • Journal Title: Adv. Opt. Mater. Volume: 10 Issue: 3 Pages: 2102034-2102034
  • DOI: 10.1002/adom.202102034
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Recycling of triplets into singlets for high-performance organic lasers (2021)
  • Author(s): Chathuranganie A. M. Senevirathne, Seiya Yoshida, Morgan Auffray, Buddhika S. B. Karunathilaka, Kenichi Goushi, Atula S. D. Sandanayake, Toshinori Matsushima*, and Chihaya Adachi*
  • Journal Title: Advanced Optical Materials Volume: 10 Issue: 1 Pages: 2101302-2101302
  • DOI: 10.1002/adom.202101302
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Enhanced light-matter interaction and polariton relaxation by the control of molecular orientation (2021)
  • Author(s): T. Ishii, F. Bencheikh, S. Forget, S. Chenais, B. Heinrich, D. Kreher, L. S. Vargas, K. Miyata, K. Onda, T. Fujihara, S. Kena-Cohen, F. Mathevet, C. Adachi
  • Journal Title: Adv. Opt. Mater. Volume: 10 Issue: 22 Pages: 2101048-2101048
  • DOI: 10.1002/adom.202101048
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] 2,6‐Dicarbonitrile Diphenyl‐1λ5 ‐Phosphinine (DCNP) A Robust Conjugated Building Block for Multi‐Functional Dyes Exhibiting Tunable Amplified Spontaneous Emission (2021)
  • 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
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Electron‐Affinity Substituent in 2,6‐Dicarbonitrile Diphenyl‐1λ5‐Phosphinine Towards High‐Quality Organic Lasing and Electroluminescence under High Current Injection (2021)
  • Author(s): Tang Xun、Balijapalli Umamahesh、Okada Daichi、Karunathilaka Buddhika S. B.、Senevirathne Chathuranganie A. M.、Lee Yi‐Ting、Feng Zhao、Sandanayaka Atula S. D.、Matsushima Toshinori、Adachi Chihaya
  • Journal Title: Advanced Functional Materials Volume: 31 Issue: 43 Pages: 2104529-2104529
  • DOI: 10.1002/adfm.202104529
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Exact Solution of Kinetic Analysis for Thermally Activated Delayed Fluorescence Materials (2021)
  • Author(s): Tsuchiya, Y., Diesing, S., Bencheikh, F., Wada, Y., dos Santos, PL., Kaji, H., Zysman-Colman, E., Samuel, IDW. and Adachi, C.
  • Journal Title: J. Phys. Chem. A Volume: 125 Issue: 36 Pages: 8074-8089
  • DOI: 10.1021/acs.jpca.1c04056
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Tetrabenzo[a,c]phenazine Backbone for Highly Efficient Orange-Red Thermally Activated Delayed Fluorescence with Completely Horizontal Molecular Orientation (2021)
  • 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
  • Peer Reviewed
• [Journal Article] Organic photostimulated luminescence associated with persistent spin-correlated radical pairs (2021)
  • Author(s): Sakurai Manabu、Kabe Ryota、Fuki Masaaki、Lin Zesen、Jinnai Kazuya、Kobori Yasuhiro、Adachi Chihaya、Tachikawa Takashi
  • Journal Title: Communications Materials Volume: 2 Issue: 1 Pages: 74-74
  • DOI: 10.1038/s43246-021-00178-3
  • NAID: 120007124098
  • Peer Reviewed / Open Access
• [Journal Article] Active Control of Spontaneous Orientation Polarization of Tris(8-hydroxyquinolinato)aluminum (Alq3) Films and Its Effect on Performance of Organic Light-Emitting Diodes (2021)
  • Author(s): Yu Esaki, Masaki Tanaka, Toshinori Matsushima, and Chihaya Adachi*
  • Journal Title: Advanced Electronic Materials Volume: 7 Issue: 9 Pages: 2100486-2100486
  • DOI: 10.1002/aelm.202100486
  • Peer Reviewed
• [Journal Article] Amplified spontaneous emission from oligo(p-phenylenevinylene) derivatives (2021)
  • Author(s): Mamada Masashi、Nakanotani Hajime、Adachi Chihaya
  • Journal Title: Materials Advances Volume: 2 Issue: 12 Pages: 3906-3914
  • DOI: 10.1039/d0ma00756k
  • Peer Reviewed
• [Journal Article] Markedly Improved Performance of Optically Pumped Organic Lasers with Two-Dimensional Distributed-Feedback Gratings (2021)
  • Author(s): Chathuranganie A. M. Senevirathne, Atula S. D. Sandanayaka*, Buddhika S. B. Karunathilaka, Takashi Fujihara, Fatima Bencheikh, Chuanjiang Qin, Kenichi Goushi, Toshinori Matsushima*, and Chihaya Adachi*
  • Journal Title: ACS Photonics Volume: 8 Issue: 5 Pages: 1324-1334
  • DOI: 10.1021/acsphotonics.0c01728
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Long‐Persistent Luminescence from an Exciplex‐Based Organic Light‐Emitting Diode (2021)
  • Author(s): Tan Shinichi、Jinnai Kazuya、Kabe Ryota、Adachi Chihaya
  • Journal Title: Advanced Materials Volume: 33 Issue: 23 Pages: 2008844-2008844
  • DOI: 10.1002/adma.202008844
  • Peer Reviewed
• [Journal Article] Thermally Activated Delayed Fluorescence Properties of Trioxoazatriangulene Derivatives Modified with Electron Donating Groups (2021)
  • Author(s): Youichi Tsuchiya; Yuma Ishikawa; Sang-Hoon Lee; Xian-Kai Chen; Jean-Luc Bredas; Hajime Nakanotani; Chihaya Adachi
  • Journal Title: Advanced Optical Materials, Volume: 9 Issue: 14 Pages: 2002174-2002174
  • DOI: 10.1002/adom.202002174
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Investigating HOMO Energy Levels of Terminal Emitters for Realizing High-Brightness and Stable TADF-Assisted Fluorescence Organic Light-Emitting Diodes (2021)
  • Author(s): Yi-Ting Lee; Chin-Yiu Chan; Masaki Tanaka; Masashi Mamada; Umamahesh Balijapalli; Youichi Tsuchiya; Hajime Nakanotani; Takuji Hatakeyama; Chihaya Adachi
  • Journal Title: Advanced Electronic Materials Volume: 7 Issue: 4 Pages: 2001090-2001090
  • DOI: 10.1002/aelm.202001090
  • Peer Reviewed
• [Journal Article] Thermally-activated Delayed Fluorescence for Light-emitting Devices (2021)
  • Author(s): Nakanotani Hajime、Tsuchiya Youichi、Adachi Chihaya
  • Journal Title: Chemistry Letters Volume: 50 Issue: 5 Pages: 938-948
  • DOI: 10.1246/cl.200915
  • NAID: 130008040396
  • Peer Reviewed / Open Access
• [Journal Article] Advantages of naphthalene as a building block for organic solid state laser dyes: smaller energy gaps and enhanced stability (2021)
  • Author(s): Oyama Yuya、Mamada Masashi、Kondo Akihiro、Adachi Chihaya
  • Journal Title: Journal of Materials Chemistry C Volume: 9 Issue: 12 Pages: 4112-4118
  • DOI: 10.1039/d0tc05387b
  • Peer Reviewed
• [Journal Article] Isotope Effect of Host Material on Device Stability of Thermally Activated Delayed Fluorescence Organic Light‐Emitting Diodes (2021)
  • Author(s): Xuelong Liu; Chin-Yiu Chan; Fabrice Mathevet; Masashi Mamada; Youichi Tsuchiya; Yi-Ting Lee; Hajime Nakanotani; Shinichiro Kobayashi; Masayuki Shiochi; Chihaya Adachi
  • Journal Title: Small Science Volume: 1, 4 Issue: 4 Pages: 2000057-2000057
  • DOI: 10.1002/smsc.202000057
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Highly Efficient Near‐Infrared Electrofluorescence from a Thermally Activated Delayed Fluorescence Molecule (2021)
  • Author(s): Balijapalli Umamahesh、Nagata Ryo、Yamada Nishiki、Nakanotani Hajime、Tanaka Masaki、D'Al?o Anthony、Placide Virginie、Mamada Masashi、Tsuchiya Youichi、Adachi Chihaya
  • Journal Title: Angewandte Chemie International Edition Volume: 60 Issue: 15 Pages: 8477-8482
  • DOI: 10.1002/anie.202016089
  • Peer Reviewed
• [Journal Article] Stable pure-blue hyperfluorescence organic light-emitting diodes with high-efficiency and narrow emission (2021)
  • Author(s): Chin-Yiu Chan; Masaki Tanaka; Yi-Ting Lee; Yiu-Wing Wong; Hajime Nakanotani; Takuji Hatakeyama; Chihaya Adachi
  • Journal Title: Nat. Photonics Volume: 15 Issue: 3 Pages: 203-207
  • DOI: 10.1038/s41566-020-00745-z
  • Peer Reviewed
• [Journal Article] Intramolecular‐Locked High Efficiency Ultrapure Violet‐Blue (CIE‐y <0.046) Thermally Activated Delayed Fluorescence Emitters Exhibiting Amplified Spontaneous Emission (2021)
  • Author(s): Aziz Khan; Xun Tang; Cheng Zhong; Qiang Wang; Sheng-Yi Yang; Fan-Cheng Kong; Shuai Yuan; Atula Sandanayaka; Chihaya Adachi; Zuo-Quan Jiang; Liang-Sheng Liao
  • Journal Title: Advanced Functional Materials Volume: 31 Issue: 15 Pages: 2009488-2009488
  • DOI: 10.1002/adfm.202009488
  • Peer Reviewed / Int'l Joint Research
• [Presentation] Intramolecular triplet-triplet annihilation up-conversion in organic light-emitting diodes (2022)
  • Author(s): 合志 憲一
  • Organizer: ICONO13 / ICOPE2022
  • Int'l Joint Research
• [Presentation] Investigation of charge transport properties in a Dion－Jacobson-type 2D organic-inorganic perovskite (2022)
  • Author(s): Xuelong Liu、安達千波矢
  • Organizer: The 83rd JSAP Autumn Meeting 2022
  • Int'l Joint Research