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Organic Semiconductor spinorbitronics

Research Project

Project/Area Number 20H00387
Research Category

Grant-in-Aid for Scientific Research (A)

Allocation TypeSingle-year Grants
Section一般
Review Section Medium-sized Section 35:Polymers, organic materials, and related fields
Research InstitutionThe University of Tokyo

Principal Investigator

渡邉 峻一郎  東京大学, 大学院新領域創成科学研究科, 准教授 (40716718)

Co-Investigator(Kenkyū-buntansha) 下位 幸弘  筑波大学, 数理物質系, 研究員 (70357226)
岡本 敏宏  東京工業大学, 物質理工学院, 教授 (80469931)
中野谷 一  九州大学, 工学研究院, 准教授 (90633412)
Project Period (FY) 2020-04-01 – 2025-03-31
Project Status Granted (Fiscal Year 2024)
Budget Amount *help
¥45,370,000 (Direct Cost: ¥34,900,000、Indirect Cost: ¥10,470,000)
Fiscal Year 2024: ¥3,120,000 (Direct Cost: ¥2,400,000、Indirect Cost: ¥720,000)
Fiscal Year 2023: ¥8,190,000 (Direct Cost: ¥6,300,000、Indirect Cost: ¥1,890,000)
Fiscal Year 2022: ¥9,100,000 (Direct Cost: ¥7,000,000、Indirect Cost: ¥2,100,000)
Fiscal Year 2021: ¥8,580,000 (Direct Cost: ¥6,600,000、Indirect Cost: ¥1,980,000)
Fiscal Year 2020: ¥16,380,000 (Direct Cost: ¥12,600,000、Indirect Cost: ¥3,780,000)
Keywords有機半導体 / スピントロニクス / スピン軌道相互作用
Outline of Research at the Start

スピン軌道相互作用 (Spin-orbit coupling: SOC)は電子スピンと電子の軌道運動の相互作用であり、固体中で電子が実効的に感じる有効磁場である。近年、SOCを起源とする新規な機能性が開拓され、「スピンオービトロニクス」という新しい学理が構築されつつある。本研究では、有機半導体分子におけるSOCの基礎学理の構築を基盤とし、SOCを分子レベルでの制御を目指す。高効率スピン電荷変換・超ロバストスピン輸送といった革新的な機能性を実現する。合成化学・固体物理学・デバイス工学を相補的に組み合わせた「有機スピンオービトロニクス」の学理を創生する。

Outline of Annual Research Achievements

本研究では、有機半導体におけるスピン軌道相互作用(SOC)の「制御」・「理解」・「機能化」を三位一体とし、スピンオービトロニクスを基盤とした革新的電子スピンデバイスの創成を目指す。SOCはスピン磁気モーメントと電子の軌道運動が生み出す磁場の相互作用である。無機個体におけるSOCの研究は古くから行われているものの、軽元素から構成される有機固体におけるSOCは意味だに未解明な部分も多い。本研究では、適切にSOC制御されたヘテロアセン分子群を用いて、革新的な電子スピンデバイス実装の足がかりとなる基盤研究を遂行してきた。ここでは、合成化学・凝縮系固体物理学・デバイス工学を包括的に組み合わせることでのみ実現する有機スピンオービトロニクスの学理を整備し、有機半導体ならではのフレキシビリティや低温・塗布プロセスの強みを活かした革新的な基盤技術・マテリアルサイエンスへと展開する。 研究四年次では、スピン磁化率の温度依存性から高密度キャリア下の電子状態計測を進めると同時に、SOCの理論的なアプローチは密度汎関数計算をベースに下位幸弘と共に行った。極低温における磁気抵抗効果からSOCの強さを電気的に決定することが可能となり、顕著な成果が得られつつある。岡本・中野谷らの合成チームとの連携も進み、スピン緩和の原因となるプロトンを排除した重水素化ヘテロアセン系材料の開発も進みつつある。100mK程度までの極低温における磁気輸送特性計測および、共通利用施設を用いた80 T程度までの強磁場実験から、有機二次元電子系における量子振動の計測などの新奇な電子状態も発見されつつある。

Current Status of Research Progress
Current Status of Research Progress

3: Progress in research has been slightly delayed.

Reason

研究四年次では、初年度から継続して立ち上げてきた物性計測手法の開発が概ね達成され、合成チーム・理論チームとの連携も進みつつあり、最終年に向けた準備がようやく整備されたと言える。また、微細加工プロセスにも進捗が見られ、スピンデバイスの製造も可能となっている。一方で、合成チームとの共同で進めているSOC変調材料に関しては、結晶薄膜の製造が困難であるなどの課題が残り、デバイス化に至る道筋が立っていない。電子スピン共鳴などの分光手法を改良し、多結晶薄膜においてもSOCの定量化が可能な方法論を見出しつつあるため、最終年に向けて課題解決が可能であると期待している。

Strategy for Future Research Activity

研究最終年次には、スピン軌道相互作用の低温物性測定および理論計算を継続して実施する。低温物性測定では、実施者が保有する無冷媒型クライオスタットを用いた磁気輸送計測に加えて、電子スピン共鳴などの分光計測を合わせて実施する。実デバイスでより重要となる固体中のSOCの評価を磁気輸送特性から実施する予定である。スピン軌道相互作用に由来する特徴的な磁場応答特性や低温輸送特性も引き続き評価する予定である。100mK程度までの極低温実験や80Tまでの強磁場実験も可能となったため新規機能性開拓にも突破口が見えている。デバイス製造に関しては、電子線リソグラフィを利用したメゾスコピックデバイスの製造プロセスも確立しつつある。

Report

(5 results)
  • 2023 Annual Research Report
  • 2022 Annual Research Report
  • 2021 Annual Research Report
  • 2020 Comments on the Screening Results   Annual Research Report
  • Research Products

    (30 results)

All 2024 2023 2022 2021 2020

All Journal Article (29 results) (of which Int'l Joint Research: 9 results,  Peer Reviewed: 29 results,  Open Access: 21 results) Presentation (1 results) (of which Int'l Joint Research: 1 results,  Invited: 1 results)

  • [Journal Article] All‐Carbon‐Based Complementary Integrated Circuits2024

    • Author(s)
      Watanabe Kazuyoshi、Miura Naoki、Taguchi Hiroaki、Komatsu Takeshi、Aratake Atsushi、Makita Tatsuyuki、Tanabe Masahiro、Wakimoto Takahiro、Kumagai Shohei、Okamoto Toshihiro、Watanabe Shun、Takeya Jun
    • Journal Title

      Advanced Materials Technologies

      Volume: 9 Issue: 5 Pages: 1673-1684

    • DOI

      10.1002/admt.202301673

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] 17.4 Environmentally-Friendly Disposable Circuit and Battery System for Reducing Impact of E-Wastes2024

    • Author(s)
      Miura Naoki、Taguchi Hiroaki、Watanabe Kazuyoshi、Nohara Masaya、Makita Tatsuyuki、Tanabe Masahiro、Wakimoto Takahiro、Kumagai Shohei、Nosaka Hideyuki、Aratake Atsushi、Okamoto Toshihiro、Watanabe Shun、Takeya Jun、Komatsu Takeshi
    • Journal Title

      IEEE International Solid-State Circuits Conference (ISSCC),

      Volume: 1 Pages: 320-323

    • DOI

      10.1109/isscc49657.2024.10454497

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Doping of molecular semiconductors through proton-coupled electron transfer2023

    • Author(s)
      Masaki Ishii, Yu Yamashita*, Shun Watanabe, Katsuhiko Ariga & Jun Takeya
    • Journal Title

      Nature

      Volume: 622 Issue: 7982 Pages: 285-291

    • DOI

      10.1038/s41586-023-06504-8

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Employment of Alkoxy Sidechains in Semicrystalline Semiconducting Polymers for Ambient-Stable p-Doped Conjugated Polymers2023

    • Author(s)
      Tadanori Kurosawa, Yu Yamashita, Yuki Kobayashi, Craig P. Yu, Shohei Kumagai, Tsubasa Mikie, Itaru Osaka, Shun Watanabe, Jun Takeya, and Toshihiro Okamoto*
    • Journal Title

      Macromolecules

      Volume: 57 Issue: 1 Pages: 328-338

    • DOI

      10.1021/acs.macromol.3c00211

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Individual and synergetic charge transport properties at the solid and electrolyte interfaces of a single ultrathin single crystal of organic semiconductors2023

    • Author(s)
      Taehyun Won , Shohei Kumagai* , Naotaka Kasuya* , Yu Yamashita , Shun Watanabe , Toshihiro Okamoto and Jun Takeya*
    • Journal Title

      Phys. Chem. Chem. Phys.

      Volume: 25 Issue: 20 Pages: 14496-14501

    • DOI

      10.1039/d3cp00782k

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] High-speed hybrid complementary ring oscillators based on solution-processed organic and amorphous metal oxide semiconductors2023

    • Author(s)
      X. Wei, S. Kumagai, T. Makita, K. Tsuzuku, A. Yamamura, M. Sasaki, S. Watanabe, and J. Takeya
    • Journal Title

      Commun Mater

      Volume: 4, 4 Issue: 1 Pages: 1-9

    • DOI

      10.1038/s43246-023-00331-0

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Electrostatically-sprayed carbon electrodes for high performance organic complementary circuits2022

    • Author(s)
      K. Watanabe, N. Miura, H. Taguchi, T. Komatsu, H. Nosaka, T. Okamoto, S. Watanabe, and J. Takeya
    • Journal Title

      Sci Rep

      Volume: 12, 16009 Issue: 1 Pages: 1-8

    • DOI

      10.1038/s41598-022-19387-y

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Improvement of contact resistance at carbon electrode/organic semiconductor interfaces through chemical doping2022

    • Author(s)
      K. Watanabe, N. Miura, H. Taguchi, T. Komatsu, H. Nosaka, T. Okamoto, Y. Yamashita, S. Watanabe, and J. Takeya
    • Journal Title

      Appl. Phys. Express

      Volume: 15 101005 Issue: 10 Pages: 1-5

    • DOI

      10.35848/1882-0786/ac92c0

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Scattering mechanism of hole carriers in organic molecular semiconductors deduced from analyses of terahertz absorption spectra using Drude-Anderson model2022

    • Author(s)
      Y. Han, T. Miyamoto, T. Otaki, N. Takamura, N. Kida, N. Osakabe, J. Tsurumi, S. Watanabe, T. Okamoto, J. Takeya and H. Okamoto
    • Journal Title

      Applied Physics Letters

      Volume: 120 Issue: 5 Pages: 053302-053302

    • DOI

      10.1063/5.0073133

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Doped semiconducting polymer nanoantennas for tunable organic plasmonics2022

    • Author(s)
      A. Karki, Y. Yamashita, SZ. Chen, T. Kurosawa, J. Takeya, V. Stanishev, V. Darakchieva, S. Watanabe, and MP. Jonsson
    • Journal Title

      Communications Materials

      Volume: 3,48 Issue: 1 Pages: 1-8

    • DOI

      10.1038/s43246-022-00268-w

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Phonon dispersion of the organic semiconductor rubrene2022

    • Author(s)
      K. Takada, K. Yoshimi, S. Tsutsui, K. Kimura, K. Hayashi, I. Hamada, S. Yanagisawa, N. Kasuya, S. Watanabe, J. Takeya, and Y. Wakabayashi
    • Journal Title

      Phys. Rev. B

      Volume: 105, 205205 Issue: 20 Pages: 1-8

    • DOI

      10.1103/physrevb.105.205205

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] “Nitrogen-Containing Perylene Diimides: Molecular Design, Robust Aggregated Structures, and Advances in n-Type Organic Semiconductors”2022

    • Author(s)
      Shohei Kumagai, Hiroyuki Ishii, Go Watanabe, Craig P. Yu, Shun Watanabe, Jun Takeya, and Toshihiro Okamoto
    • Journal Title

      Acc. Chem. Res.

      Volume: 55 Issue: 5 Pages: 660-672

    • DOI

      10.1021/acs.accounts.1c00548

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] ”Scalable printing of two-dimensional single crystals of organic emiconductors towards high-end device applications”2022

    • Author(s)
      S. Kumagai, T. Makita, S. Watanabe, and J. Takeya
    • Journal Title

      Appl. Phys. Express

      Volume: 15 Issue: 3 Pages: 030101-030101

    • DOI

      10.35848/1882-0786/ac435a

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Band mobility exceeding 10cm2V-1s-1 assessed by field-effect and chemical double doping in semicrystalline polymeric semiconductors2021

    • Author(s)
      Ito Masato、Yamashita Yu、Mori Taizo、Ariga Katsuhiko、Takeya Jun、Watanabe Shun
    • Journal Title

      Applied Physics Letters

      Volume: 119 Issue: 1 Pages: 013302-013302

    • DOI

      10.1063/5.0052279

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Highly air-stable, n-doped conjugated polymers achieved by dimeric organometallic dopants2021

    • Author(s)
      Yamashita Yu、Jhulki Samik、Bhardwaj Dinesh、Longhi Elena、Kumagai Shohei、Watanabe Shun、Barlow Stephen、Marder Seth R.、Takeya Jun
    • Journal Title

      Journal of Materials Chemistry C

      Volume: 9 Issue: 12 Pages: 4105-4111

    • DOI

      10.1039/d0tc05931e

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Hyper 100 °C Langmuir-Blodgett (Langmuir-Schaefer) Technique for Organized Ultrathin Film of Polymeric Semiconductors2021

    • Author(s)
      Ito Masato、Yamashita Yu、Mori Taizo、Chiba Masaaki、Futae Takayuki、Takeya Jun、Watanabe Shun、Ariga Katsuhiko
    • Journal Title

      Langmuir

      Volume: 38 Issue: 17 Pages: 5237-5247

    • DOI

      10.1021/acs.langmuir.1c02596

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] ”Two-dimensional hole gas in organic semiconductors”2021

    • Author(s)
      N. Kasuya, J. Tsurumi, T. Okamoto, S. Watanabe, and J. Takeya
    • Journal Title

      Nat. Mater.

      Volume: 20 Issue: 10 Pages: 1401-1406

    • DOI

      10.1038/s41563-021-01074-4

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] ”Stabilizing solution-processed metal oxide thin-film transistors via trilayer organic-inorganic hybrid passivation”2021

    • Author(s)
      X. Wei, S. Kumagai, M. Sasaki, S. Watanabe, J. Takeya
    • Journal Title

      AIP Advances

      Volume: 11 Issue: 3 Pages: 035027-035027

    • DOI

      10.1063/5.0038128

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Supramolecular cocrystals built through redox-triggered ion intercalation in π-conjugated polymers2021

    • Author(s)
      Yamashita Yu、Tsurumi Junto、Kurosawa Tadanori、Ueji Kan、Tsuneda Yukina、Kohno Shinya、Kempe Hideto、Kumagai Shohei、Okamoto Toshihiro、Takeya Jun、Watanabe Shun
    • Journal Title

      Communications Materials

      Volume: 2 Issue: 1 Pages: 45-45

    • DOI

      10.1038/s43246-021-00148-9

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Nano‐Ground Glass as a Superhydrophilic Template for Printing High‐Performance Organic Single‐Crystal Thin Films2021

    • Author(s)
      Makita Tatsuyuki、Ninomiya Yoma、Kumagai Shohei、Okamoto Toshihiro、Sasaki Mari、Watanabe Shun、Takeya Jun
    • Journal Title

      Advanced Materials Interfaces

      Volume: in press Issue: 10 Pages: 2100033-2100033

    • DOI

      10.1002/admi.202100033

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Thermally-activated Delayed Fluorescence for Light-emitting Devices2021

    • 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

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Surface Doping of Organic Single‐Crystal Semiconductors to Produce Strain‐Sensitive Conductive Nanosheets2020

    • Author(s)
      Watanabe Shun、Hakamatani Ryohei、Yaegashi Keita、Yamashita Yu、Nozawa Han、Sasaki Mari、Kumagai Shohei、Okamoto Toshihiro、Tang Cindy G.、Chua Lay‐Lay、Ho Peter K. H.、Takeya Jun
    • Journal Title

      Advanced Science

      Volume: 8 Issue: 3 Pages: 2002065-2002065

    • DOI

      10.1002/advs.202002065

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Cooperative Aggregations of Nitrogen-Containing Perylene Diimides Driven by Rigid and Flexible Functional Groups2020

    • Author(s)
      S. Kumagai, H. Ishii, G. Watanabe, T. Annaka, E. Fukuzaki, Y. Tani, H. Sugiura, T. Watanabe, T. Kurosawa, J. Takeya, and T. Okamoto
    • Journal Title

      Chem. Mater.

      Volume: 32 Issue: 21 Pages: 9115-9125

    • DOI

      10.1021/acs.chemmater.0c01888

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Band-like transporting and thermally durable V-shaped organic semiconductors with a phenyl key block2020

    • Author(s)
      C. Sawabe, S. Kumagai, M. Mitani, H. Ishii, M. Yamagishi, H. Sagayama, R. Kumai, H. Sato, J. Takeya and T. Okamoto
    • Journal Title

      J. Mater. Chem. C,

      Volume: 8 Issue: 40 Pages: 14172-14179

    • DOI

      10.1039/d0tc03318a

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Correlation between the static and dynamic responses of organic single-crystal field-effect transistors2020

    • Author(s)
      Sawada Taiki、Yamamura Akifumi、Sasaki Mari、Takahira Kayo、Okamoto Toshihiro、Watanabe Shun、Takeya Jun
    • Journal Title

      Nature Communications

      Volume: 11 Issue: 1 Pages: 1-7

    • DOI

      10.1038/s41467-020-18616-0

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Alkyl-Substituted Selenium-Bridged V-Shaped Organic Semiconductors Exhibiting High Hole Mobility and Unusual Aggregation Behavior2020

    • Author(s)
      Okamoto Toshihiro、Mitani Masato、Yu Craig P.、Mitsui Chikahiko、Yamagishi Masakazu、Ishii Hiroyuki、Watanabe Go、Kumagai Shohei、Hashizume Daisuke、Tanaka Shota、Yano Masafumi、Kushida Tomokatsu、Sato Hiroyasu、Sugimoto Kunihisa、Kato Takashi、Takeya Jun
    • Journal Title

      Journal of the American Chemical Society

      Volume: 142 Issue: 35 Pages: 14974-14984

    • DOI

      10.1021/jacs.0c05522

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Electroless‐Plated Gold Contacts for High‐Performance, Low Contact Resistance Organic Thin Film Transistors2020

    • Author(s)
      Makita Tatsuyuki、Nakamura Ryohei、Sasaki Mari、Kumagai Shohei、Okamoto Toshihiro、Watanabe Shun、Takeya Jun
    • Journal Title

      Advanced Functional Materials

      Volume: 30 Issue: 39 Pages: 2003977-2003977

    • DOI

      10.1002/adfm.202003977

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Effect of Electronically Distinct Aromatic Substituents on the Molecular Assembly and Hole Transport of V-Shaped Organic Semiconductors2020

    • Author(s)
      Yu Craig P.、Mitani Masato、Ishii Hiroyuki、Yamagishi Masakazu、Kitamura Hiroki、Yano Masafumi、Takeya Jun、Okamoto Toshihiro
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 124 Issue: 32 Pages: 17503-17511

    • DOI

      10.1021/acs.jpcc.0c04088

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Robust, high-performance n-type organic semiconductors2020

    • Author(s)
      T. Okamoto, S. Kumagai, E Fukuzaki, H. Ishii, G. Watanabe, N. Niitsu, T. Annaka, M. Yamagishi, Y. Tani, H. Sugiura, T. Watanabe, S. Watanabe, and J. Takeya
    • Journal Title

      Sci. Adv.

      Volume: 6 Issue: 18

    • DOI

      10.1126/sciadv.aaz0632

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Presentation] Metallic polymers mediated by molecules, ions, and their interstices2023

    • Author(s)
      Shun Watanabe
    • Organizer
      The 13th SPSJ International Polymer Conference
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited

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Published: 2020-04-28   Modified: 2024-12-25  

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