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Development of a Simple and Scalable Method for Organic Semiconductor Single Crystal Growth and Formation of Multi-Single Crystal Thin Films for Applications in Field-Effect Transistor-Based Devices.

Research Project

Project/Area Number 22K14293
Research Category

Grant-in-Aid for Early-Career Scientists

Allocation TypeMulti-year Fund
Review Section Basic Section 21050:Electric and electronic materials-related
Research InstitutionInstitute of Physical and Chemical Research

Principal Investigator

Bulgarevich Kirill  国立研究開発法人理化学研究所, 創発物性科学研究センター, 特別研究員 (60880268)

Project Period (FY) 2022-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥4,550,000 (Direct Cost: ¥3,500,000、Indirect Cost: ¥1,050,000)
Fiscal Year 2023: ¥910,000 (Direct Cost: ¥700,000、Indirect Cost: ¥210,000)
Fiscal Year 2022: ¥3,640,000 (Direct Cost: ¥2,800,000、Indirect Cost: ¥840,000)
Keywords有機半導体 / 有機トランジスタ / 単結晶 / 薄膜 / 多単結晶膜 / 大面積 / 間接昇華法 / 間接昇華 / 単結晶有機半導体 / 大気圧下蒸着 / 大気圧蒸着
Outline of Research at the Start

The proposed research aims to develop a simple, scalable, and vacuum and solution free method for growth and transfer of organic semiconductor single crystals (SCs) for applications in high-performance devices based on organic field-effect transistors (OFETs). A method is proposed to cover entire substrate surface with SCs as Multi-SC films. Such films may have similar applications in OFET-based devices as solution grown thin-films, but can show better performance. Thus, practical applications will be offered to organic semiconductor SCs which are mainly used for studying intrinsic properties.

Outline of Final Research Achievements

We developed a novel crystal growth technique named "indirect sublimation", and successfully formed organic semiconductor single-crystals on large-area without the use of vacuum or solvents. These numerous freestanding single-crystals were transferred onto device substrates through a simple press-transfer and rubbing process, creating a so-called "multi-single-crystal (MSC)" film, where small crystals overlap to cover large areas. We confirmed that organic field-effect transistors (OFETs) using this MSC film as the active layer perform similarly to single-crystal devices. By combining such OFETs, we successfully fabricated pseudo-CMOS devices that exhibit inverter characteristics similar to CMOS devices. Furthermore, using our unique crystal structure simulation algorithm, we successfully developed a novel ultra-high mobility organic semiconductor material, which also has potential for MSC film applications.

Academic Significance and Societal Importance of the Research Achievements

新たに開発された「間接昇華法」および「多単結晶膜」形成は真空や溶媒を用いずに有機半導体の大面積な結晶性薄膜を形成する手法である。特に我々が最近報告した有機半導体MT-ピレンは多単結晶膜トランジスタで(>15 cm2 V-1 s-1)の非常に高い移動度を示し、この技術により環境への影響を抑えた高性能な有機デバイスの実現が期待される。さらに、我々が独自で開発した結晶構造シミュレーションアルゴリズムを使用することでMT-ピレンと同等な移動度を示す新規材料が開発された。この手法は多単結晶膜応用を念頭に置いた溶解性にとらわれない材料設計と構造シミュレーションによる効率的な高移動度新規材料開発につながる。

Report

(3 results)
  • 2023 Annual Research Report   Final Research Report ( PDF )
  • 2022 Research-status Report
  • Research Products

    (18 results)

All 2024 2023 2022

All Journal Article (8 results) (of which Int'l Joint Research: 3 results,  Peer Reviewed: 8 results,  Open Access: 4 results) Presentation (9 results) (of which Int'l Joint Research: 2 results) Book (1 results)

  • [Journal Article] Crystal-Structure Control of Molecular Semiconductors by Methylthiolation: Toward Ultrahigh Mobility2024

    • Author(s)
      Takimiya Kazuo、Bulgarevich Kirill、Kawabata Kohsuke
    • Journal Title

      Accounts of Chemical Research

      Volume: 57 Issue: 6 Pages: 884-894

    • DOI

      10.1021/acs.accounts.3c00756

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Crystal‐Structure Simulation of Methylthiolated <i>Peri</i>‐Condensed Polycyclic Aromatic Hydrocarbons for Identifying Promising Molecular Semiconductors: Discovery of 1,3,8,10‐tetrakis(methylthio)peropyrene Showing Ultrahigh Mobility2023

    • Author(s)
      Bulgarevich Kirill、Horiuchi Shingo、Takimiya Kazuo
    • Journal Title

      Advanced Materials

      Volume: 35 Issue: 49 Pages: 2305548-2305548

    • DOI

      10.1002/adma.202305548

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Contrasted behaviours of methylthiolated perylene and pyrene as organic semiconductors: implications of molecular electronic structure and crystal structure2023

    • Author(s)
      Takimiya Kazuo、Bulgarevich Kirill、Horiuchi Singo
    • Journal Title

      Journal of Materials Chemistry C

      Volume: 11 Issue: 32 Pages: 10809-10815

    • DOI

      10.1039/d3tc02063k

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Crystal-structure simulation of molecular semiconductors: brickwork-related crystal structures of methylthiolated <i>peri</i>-condensed polycyclic aromatic hydrocarbons2023

    • Author(s)
      Bulgarevich Kirill、Takimiya Kazuo
    • Journal Title

      Materials Horizons

      Volume: 10 Issue: 12 Pages: 5492-5499

    • DOI

      10.1039/d3mh01055d

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Bandlike versus Temperature-Independent Carrier Transport in Isomeric Diphenyldinaphtho[2,3-b:2′,3′-f]thieno[3,2-b]thiophenes2022

    • Author(s)
      Takimiya Kazuo、Bulgarevich Kirill、Horiuchi Shingo、Sato Aoi、Kawabata Kohsuke
    • Journal Title

      ACS Materials Letters

      Volume: 4 Issue: 4 Pages: 675-681

    • DOI

      10.1021/acsmaterialslett.2c00084

    • Related Report
      2022 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] 1,3,6,8-Tetrakis(methylchalcogeno)pyrenes: Effects of Chalcogen Atoms on the Crystal Structure and Transport Properties2022

    • Author(s)
      Bulgarevich Kirill、Horiuchi Shingo、Ogaki Takuya、Takimiya Kazuo
    • Journal Title

      Chemistry of Materials

      Volume: 34 Issue: 14 Pages: 6606-6616

    • DOI

      10.1021/acs.chemmater.2c01544

    • Related Report
      2022 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] What Defines a Crystal Structure? Effects of Chalcogen Atoms in 3, <scp>7‐Bis</scp> (methylchalcogeno)benzo[1,2‐ <i>b</i> :4,5‐ <i>b</i> ′] <scp>dichalcogenophene‐Based</scp> Organic Semiconductors <sup>†</sup>2022

    • Author(s)
      Takimiya Kazuo、Bulgarevich Kirill、Sahara Kamon、Kanazawa Kiseki、Takenaka Hiroyuki、Kawabata Kohsuke
    • Journal Title

      Chinese Journal of Chemistry

      Volume: 40 Issue: 21 Pages: 2546-2558

    • DOI

      10.1002/cjoc.202200302

    • Related Report
      2022 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Uncovered Effects of thieno[2,3-<i>b</i>]thiophene Substructure in a Tetrathienoacene Backbone: Reorganization Energy and Intermolecular Interaction2022

    • Author(s)
      Kanazawa Kiseki、Bulgarevich Kirill、Kawabata Kohsuke、Takimiya Kazuo
    • Journal Title

      Chemistry of Materials

      Volume: 35 Issue: 1 Pages: 280-288

    • DOI

      10.1021/acs.chemmater.2c03160

    • Related Report
      2022 Research-status Report
    • Peer Reviewed
  • [Presentation] Multi-Single-Crystal Films: Towards Practical Applications of Single-Crystal Organic Semiconductors2024

    • Author(s)
      Kirill Bulgarevich and Kazuo Takimiya
    • Organizer
      CEMS International Symposium on Supramolecular Chemistry and Functional Materials 2024
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 有機半導体「多単結晶膜」:単結晶デバイスの大面積化2024

    • Author(s)
      ブルガレビッチ キリル,瀧宮和男
    • Organizer
      第71回応用物理学会春季学術講演会
    • Related Report
      2023 Annual Research Report
  • [Presentation] In-silico crystallization: brickwork型構造シミュレーションの実験的確認と適用可能結晶系範囲の拡張2023

    • Author(s)
      ブルガレビッチ キリル,堀内信吾,瀧宮和男
    • Organizer
      第70回応用物理学会春季学術講演会
    • Related Report
      2023 Annual Research Report
  • [Presentation] In silico crystallization: simulation of brickwork-related crystal structures using step-by-step optimization of intermolecular interactions2023

    • Author(s)
      Kirill Bulgarevich and Kazuo Takimiya
    • Organizer
      CEMS Topical Meeting on Chemistry of π-Conjugated Materials
    • Related Report
      2023 Annual Research Report
  • [Presentation] In-silico crystallization (3): pitched pai-積層とinclined brickwork 構造の類似性とシミュレーション2023

    • Author(s)
      Kirill Bulgarevich and Kazuo Takimiya
    • Organizer
      第84回応用物理学会秋季学術講演会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Crystal Growth by “Indirect Sublimation” and Formation of Multi-Single-Crystal Films for Practical Applications of Single-Crystal Organic Semiconductors2023

    • Author(s)
      Kirill Bulgarevich and Kazuo Takimiya
    • Organizer
      The 7th Symposium for the Core Research Clusters for Materials Science and Spintronics and the 6th Symposium on International Joint Graduate Program in Materials Science and Spintronics
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] In-silico crystallization (2): brickwork型構造シミュレー ションの実験的確認と適用可能結晶系範囲の拡張2023

    • Author(s)
      Bulgarevich Dmitrievich Kirill
    • Organizer
      第70回応用物理学会春学術講演会
    • Related Report
      2022 Research-status Report
  • [Presentation] In-silico crystallization: メチルカルコゲノピレンのbrickwork型構造の計算による再現2022

    • Author(s)
      Bulgarevich Dmitrievich Kiril
    • Organizer
      第83回応用物理学会秋学術講演会
    • Related Report
      2022 Research-status Report
  • [Presentation] 高移動度有機半導体材料探索:構造-物性相関と結晶構造予測2022

    • Author(s)
      Kirill Bulgarevich
    • Organizer
      第16回物性科学領域横断研究会
    • Related Report
      2022 Research-status Report
  • [Book] 有機半導体の開発と最新動向 ~ 第8章 Brickwork型結晶構造のシミュレーションに基づく高移動度有機半導体探索2024

    • Author(s)
      Kirill Bulgarevich,瀧宮 和男
    • Total Pages
      11
    • Publisher
      シーエムシー出版
    • ISBN
      9784781317632
    • Related Report
      2023 Annual Research Report

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Published: 2022-04-19   Modified: 2025-01-30  

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