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Development of heavy-metal-free quantum dot light emitting diodes with tunable emission properties in a broad wavelength range

Research Project

Project/Area Number 21H01910
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 32020:Functional solid state chemistry-related
Research InstitutionNational Institute for Materials Science

Principal Investigator

SHIRAHATA NAOTO  国立研究開発法人物質・材料研究機構, ナノアーキテクトニクス材料研究センター, グループリーダー (80421428)

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: ¥3,900,000 (Direct Cost: ¥3,000,000、Indirect Cost: ¥900,000)
Fiscal Year 2022: ¥4,940,000 (Direct Cost: ¥3,800,000、Indirect Cost: ¥1,140,000)
Fiscal Year 2021: ¥8,840,000 (Direct Cost: ¥6,800,000、Indirect Cost: ¥2,040,000)
Keywordsナノ結晶 / 半導体量子ドット / 蛍光体 / ペロブスカイト結晶 / オプトエレクトロニクス / 発光ダイオード / フォトディテクター / 配位子工学 / シリコン量子ドット / III-V族半導体量子ドット / ダブルペロブスカイト半導体 / ハロゲン化錫ペロブスカイト半導体 / エレクトロルミネッセンス / フォトダイオード / リガンド交換 / 量子ドット / ナノ粒子 / フォトルミネッセンス / 有機無機ハイブリッド / ペロブスカイト / 外部量子収率 / 近赤外発光 / コロイダル粒子 / ルミネッセンス
Outline of Research at the Start

本研究は、次世代環境対応型発光デバイスのニューモデルとなりうる「量子ドット(QD)を活性層に具備する発光素子」創製を目的とする。応募者は、1-5nmの極狭サイズ領域においてQDの粒子径を±1.5Åレベルで制御可能な独自の湿式合成技術を基軸に、コア/シェル界面制御技術を融合することで「発光特性に優れた環境毒性のないQD」を合成する。さらに当該QDを活性層に具備する発光ダイオードを作製する。本研究を実践することで、従来の「重金属ありきのQD開発研究」に漂う閉塞感を打破し、環境QDを研究対象の軸に据えた新しい学術基盤を開拓する。

Outline of Final Research Achievements

The objective of this study was to create light emitting diodes (QLEDs) with semiconductor quantum dots (QDs) in the active layer that comply with the RoHs directive. Si, InP, Cs2Ag1-xNaxInX6 as visible phosphors, and InSb, Si, and CsSnX3 as shortwave IR phosphors were synthesized. In the Si system, the external quantum yield of 12% for EL was achieved by narrowing the distance between particles in the active layer of QLEDs. InP-based semiconductors, we discovered for the first time in III-V semiconductors that coherent core/shell structures are possible, and achieved both PLQY>70% and PL-FWHM<35nm. By elucidating the correlation between structure and luminescence, we succeeded in constructing the optimum luminescent layer for QLEDs.

Academic Significance and Societal Importance of the Research Achievements

我が国の成長戦略「グリーン社会の実現」に貢献する次世代空間映像技術を材料面で支える光源が求められている。2023年ノーベル化学賞を受賞したコロイダルQDに特徴的な狭帯化された発光スペクトルはデバイスの活性層に最適である。しかしQDの構成元素であるCd、Pb、HgがRoHSやJIGに準拠しない。このような閉塞感を打破するために、本研究課題では、従来発光層として検討されてこなかったSiをはじめ、III-V族化合物半導体、非鉛系ペロブスカイト等の半導体結晶をQD化する合成方法を開発、発光の学理探求を通じて蛍光量子収率の増強に成功、環境QDを研究対象の軸に据えた新しい学術基盤開拓へ向け第一歩となった。

Report

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

    (47 results)

All 2024 2023 2022 2021 Other

All Int'l Joint Research (3 results) Journal Article (22 results) (of which Int'l Joint Research: 6 results,  Peer Reviewed: 22 results,  Open Access: 10 results) Presentation (19 results) (of which Int'l Joint Research: 6 results,  Invited: 2 results) Book (1 results) Remarks (1 results) Patent(Industrial Property Rights) (1 results)

  • [Int'l Joint Research] University College London(英国)

    • Related Report
      2022 Annual Research Report
  • [Int'l Joint Research] KAUST(サウジアラビア)

    • Related Report
      2021 Annual Research Report
  • [Int'l Joint Research] Soochow University/Shanghai Institute of Technology/USTC(中国)

    • Related Report
      2021 Annual Research Report
  • [Journal Article] Recent Progress in Controlled Nanostructure of Colloidal Nanocrystal Powders for Efficient Light Emission2024

    • Author(s)
      Shirahata Naoto
    • Journal Title

      KONA Powder and Particle Journal

      Volume: 41 Issue: 0 Pages: 172-182

    • DOI

      10.14356/kona.2024001

    • ISSN
      0288-4534, 2187-5537
    • Year and Date
      2024-01-10
    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Rational ligand design for enhanced carrier mobility in self-powered SWIR photodiodes based on colloidal InSb quantum dots2024

    • Author(s)
      Chatterjee Subhashri、Nemoto Kazuhiro、Sun Hong-Tao、Shirahata Naoto
    • Journal Title

      Nanoscale Horizons

      Volume: 9 Issue: 5 Pages: 817-827

    • DOI

      10.1039/d4nh00038b

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Highly efficient, self-powered UV photodiodes based on leadfree perovskite nanocrystals through interfacial engineering2023

    • Author(s)
      Huang Xiaoyu、Sun Hong-Tao、Shirahata Naoto
    • Journal Title

      Nanotechnology

      Volume: 35 Issue: 3 Pages: 035701-035701

    • DOI

      10.1088/1361-6528/ad0303

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Solution-Processed UV Photodiodes Based on Cs<sub>2</sub>Ag<sub>0.35</sub>Na<sub>0.65</sub>InCl<sub>6</sub> Perovskite Nanocrystals2023

    • Author(s)
      Huang Xiaoyu、Yamada Hiroyuki、Sun Hong-Tao、Shirahata Naoto
    • Journal Title

      ACS Applied Nano Materials

      Volume: 6 Issue: 21 Pages: 20389-20397

    • DOI

      10.1021/acsanm.3c04427

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Solution-Processed InSb Quantum Dot Photodiodes for Short-Wave Infrared Sensing2023

    • Author(s)
      Chatterjee Subhashri、Nemoto Kazuhiro、Ghosh Batu、Sun Hong-Tao、Shirahata Naoto
    • Journal Title

      ACS Applied Nano Materials

      Volume: 6 Issue: 17 Pages: 15540-15550

    • DOI

      10.1021/acsanm.3c02221

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Metal?organic framework scintillators detect radioactive gases2023

    • Author(s)
      Sun Hong-Tao、Shirahata Naoto
    • Journal Title

      Nature Photonics

      Volume: 17 Issue: 8 Pages: 646-647

    • DOI

      10.1038/s41566-023-01256-3

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Mechanistic Insight into the Precursor Chemistry of Cesium Tin Iodide Perovskite Nanocrystals2023

    • Author(s)
      Zhang Bin-Bin、Chen Jia-Kai、Zhang Cong、Shirahata Naoto、Sun Hong-Tao
    • Journal Title

      ACS Materials Letters

      Volume: 5 Issue: 7 Pages: 1954-1961

    • DOI

      10.1021/acsmaterialslett.3c00413

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Impact of coherent core/shell architecture on fast response in InP-based quantum dot photodiodes2023

    • Author(s)
      Nemoto Kazuhiro、Watanabe Junpei、Yamada Hiroyuki、Sun Hong-Tao、Shirahata Naoto
    • Journal Title

      Nanoscale Advances

      Volume: 5 Issue: 3 Pages: 907-915

    • DOI

      10.1039/d2na00734g

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Photosensitizer Encryption with Aggregation Enhanced Singlet Oxygen Production2022

    • Author(s)
      Clarisse Bloyet, Flavien Sciortino, Yoshitaka Matsushita, Paul A. Karr, Anuradha Liyanage, Wipakorn Jevasuwan, Naoki Fukata, Subrata Maji, Jan Hynek, Francis D'Souza, Lok Kumar Shrestha, Katsuhiko Ariga, Tomohiko Yamazaki, Naoto Shirahata, Jonathan P. Hill, Daniel T. Payne
    • Journal Title

      Journal of the American Chemical Society

      Volume: ー Issue: 24 Pages: 10830-10843

    • DOI

      10.1021/jacs.2c02596

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Coherent InP/ZnS core@shell quantum dots with narrow-band green emissions2022

    • Author(s)
      Nemoto Kazuhiro、Watanabe Junpei、Sun Hong-Tao、Shirahata Naoto
    • Journal Title

      Nanoscale

      Volume: 14 Issue: 27 Pages: 9900-9909

    • DOI

      10.1039/d2nr02071h

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Impact of bismuth-doping on enhanced radiative recombination in lead-free double-perovskite nanocrystals2022

    • Author(s)
      Huang Xiaoyu、Matsushita Yoshitaka、Sun Hong-Tao、Shirahata Naoto
    • Journal Title

      Nanoscale Advances

      Volume: 4 Issue: 14 Pages: 3091-3100

    • DOI

      10.1039/d2na00238h

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Generating Lifetime-Enhanced Microbubbles by Decorating Shells with Silicon Quantum Nano-Dots Using a 3-Series T-Junction Microfluidic Device2022

    • Author(s)
      Wu Bingjie、Luo C. J.、Palaniappan Ashwin、Jiang Xinyue、Gultekinoglu Merve、Ulubayram Kezban、Bayram Cem、Harker Anthony、Shirahata Naoto、Khan Aaqib H.、Dalvi Sameer V.、Edirisinghe Mohan
    • Journal Title

      Langmuir

      Volume: 38 Issue: 36 Pages: 10917-10933

    • DOI

      10.1021/acs.langmuir.2c00126

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Effect of the surface coverage of an alkyl carboxylic acid monolayer on waterborne and cellular uptake behaviors for silicon quantum dots2022

    • Author(s)
      Shirahata Naoto
    • Journal Title

      Scientific Reports

      Volume: 12 Issue: 1 Pages: 17211-17211

    • DOI

      10.1038/s41598-022-21698-z

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Postproduction Approach to Enhance the External Quantum Efficiency for Red Light-Emitting Diodes Based on Silicon Nanocrystals2022

    • Author(s)
      Yamada Hiroyuki、Watanabe Junpei、Nemoto Kazuhiro、Sun Hong-Tao、Shirahata Naoto
    • Journal Title

      Nanomaterials

      Volume: 12 Issue: 23 Pages: 4314-4314

    • DOI

      10.3390/nano12234314

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Water-Soluble Silicon Quantum Dots toward Fluorescence-Guided Photothermal Nanotherapy2022

    • Author(s)
      Ozbilgin Irem Nur Gamze、Yamazaki Tomohiko、Watanabe Junpei、Sun Hong-Tao、Hanagata Nobutaka、Shirahata Naoto
    • Journal Title

      Langmuir

      Volume: 38 Issue: 17 Pages: 5188-5196

    • DOI

      10.1021/acs.langmuir.1c02326

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Phosphatidylcholine-mediated regulation of growth kinetics for colloidal synthesis of cesium tin halide nanocrystals2021

    • Author(s)
      Wang Lu-Ming、Chen Jia-Kai、Zhang Bin-Bin、Liu Qi、Zhou Yang、Shu Jie、Wang Zuoshan、Shirahata Naoto、Song Bo、Mohammed Omar F.、Bakr Osman M.、Sun Hong-Tao
    • Journal Title

      Nanoscale

      Volume: 13 Issue: 39 Pages: 16726-16733

    • DOI

      10.1039/d1nr04618g

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Theory-Guided Synthesis of Highly Luminescent Colloidal Cesium Tin Halide Perovskite Nanocrystals2021

    • Author(s)
      Liu Qi、Yin Jun、Zhang Bin-Bin、Chen Jia-Kai、Zhou Yang、Zhang Lu-Min、Wang Lu-Ming、Zhao Qing、Hou Jingshan、Shu Jie、Song Bo、Shirahata Naoto、Bakr Osman M.、Mohammed Omar F.、Sun Hong-Tao
    • Journal Title

      Journal of the American Chemical Society

      Volume: 143 Issue: 14 Pages: 5470-5480

    • DOI

      10.1021/jacs.1c01049

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Shining Light on the Structure of Lead Halide Perovskite Nanocrystals2021

    • Author(s)
      Chen Jia-Kai、Zhao Qing、Shirahata Naoto、Yin Jun、Bakr Osman M.、Mohammed Omar F.、Sun Hong-Tao
    • Journal Title

      ACS Materials Letters

      Volume: 3 Issue: 6 Pages: 845-861

    • DOI

      10.1021/acsmaterialslett.1c00197

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Silicon Quantum Dots for Light-Emitting Diodes Extending to the NIR-II Window2021

    • Author(s)
      Watanabe Junpei、Yamada Hiroyuki、Sun Hong-Tao、Moronaga Taku、Ishii Yasushi、Shirahata Naoto
    • Journal Title

      ACS Applied Nano Materials

      Volume: 4 Issue: 11 Pages: 11651-11660

    • DOI

      10.1021/acsanm.1c02223

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Metal-free scintillators excite X-ray community2021

    • Author(s)
      Chen Jia-Kai、Shirahata Naoto、Sun Hong-Tao
    • Journal Title

      Nature Photonics

      Volume: 15 Issue: 3 Pages: 171-172

    • DOI

      10.1038/s41566-020-00751-1

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Non‐Rare‐Earth UVC Persistent Phosphors Enabled by Bismuth Doping2021

    • Author(s)
      Liu Qi、Feng Zhao‐Yang、Li Hong、Zhao Qing、Shirahata Naoto、Kuroiwa Yoshihiro、Moriyoshi Chikako、Duan Chang‐Kui、Sun Hong‐Tao
    • Journal Title

      Advanced Optical Materials

      Volume: 9 Issue: 8 Pages: 2002065-2002065

    • DOI

      10.1002/adom.202002065

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Advances and Challenges in Tin Halide Perovskite Nanocrystals2021

    • Author(s)
      Chen Jia-Kai、Zhang Bin-Bin、Liu Qi、Shirahata Naoto、Mohammed Omar F.、Bakr Osman M.、Sun Hong-Tao
    • Journal Title

      ACS Materials Letters

      Volume: 3 Issue: 11 Pages: 1541-1557

    • DOI

      10.1021/acsmaterialslett.1c00444

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Presentation] インジウムアンチモン量子ドットの湿式合成と短波長赤外フォトダイオードへの応用2024

    • Author(s)
      白幡直人, Subhashri Chatterjee
    • Organizer
      日本化学会 第104春季年会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Solution Processed Nanocrystals for Bioapplications2023

    • Author(s)
      Naoto Shirahata
    • Organizer
      2023 Japan-Taiwan Nanomaterial and Biomedicine Workshop
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] InSb Quantum Dots for SWIR Photodiode2023

    • Author(s)
      Subhashri Chatterjee, Naoto Shirahata
    • Organizer
      International Conference on Powder and Powder Metallurgy 2023
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Mechanistic Insight into the Precursor Chemistry of Cesium Tin Iodide Perovskite Nanocrystals2023

    • Author(s)
      Binbin Zhang, Jiakai Chen, Cong Zhang, Naoto Shirahata, Hong-Tao Sun
    • Organizer
      International Conference on Powder and Powder Metallurgy 2023
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Colloidal Semiconductor Nanocrystals for Solution-processed Optoelectronic Applications2023

    • Author(s)
      Naoto Shirahata, Kazuhiro Nemoto, Subhashri Chatterjee
    • Organizer
      WPI-MANA International Symposium 2023
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 非鉛系ダブルペロブスカイトナノ結晶粒子の合成と発光特性2023

    • Author(s)
      白幡直人, HUANG, Xiaoyu
    • Organizer
      日本化学会第103春季年会
    • Related Report
      2023 Annual Research Report
  • [Presentation] コヒーレントコアシェル構造を有する InP/ZnSナノ結晶の合成と応用2023

    • Author(s)
      根本一宏, 白幡直人
    • Organizer
      日本化学会第103春季年会
    • Related Report
      2023 Annual Research Report
  • [Presentation] コヒーレントコアシェル構造を有するIII-V族系化合物半導体ナノ粒子の合成とフォトダイオードへの応用2023

    • Author(s)
      根本一宏, 白幡直人
    • Organizer
      粉体粉末冶金協会2023年度春季大会
    • Related Report
      2023 Annual Research Report
  • [Presentation] InP/ZnSコアシェル構造制御に基づくオプトエレトロニクス素子性能増強2023

    • Author(s)
      根本一宏, 白幡直人
    • Organizer
      日本セラミックス協会第36回秋季シンポジウム
    • Related Report
      2023 Annual Research Report
  • [Presentation] ダブルペロブスカイトナノ粒子の合成とフォトダイオード創製2023

    • Author(s)
      Xiaoyu Huang, 白幡直人
    • Organizer
      日本セラミックス協会第36回秋季シンポジウム
    • Related Report
      2023 Annual Research Report
  • [Presentation] チューナブル発光/受光材料2023

    • Author(s)
      白幡直人
    • Organizer
      NIMS材料技術展示会2023
    • Related Report
      2023 Annual Research Report
  • [Presentation] 非鉛ペロブスカイト粒子の合成とフォトダイオードの創製2023

    • Author(s)
      Xiaoyu Huang, 白幡直人
    • Organizer
      粉体粉末冶金協会2023年度秋季大会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Colloidal Synthesis of Semiconductor Quantum Dots for Optoelectronic Applications2022

    • Author(s)
      Naoto Shirahata, Hong-Tao Sun, Kazuhiro Nemoto, Xiaoyu Huang, Hiroyuki Yamada, Subhashri Chatterjee, Junpei Watanabe, Kentaro Furukoshi
    • Organizer
      WPI-MANA International Symposium 2022
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Investigation of Photothermal Response and Fluorescence Imaging of Water-soluble Silicon Quantum Dots for Theranostic Applications2022

    • Author(s)
      Irem Nur Gamze Ozbiligin, Hiroyuki Yamada, Junpei Watanabe, Tomohiko Yamazaki, Naoto Shirahata, Tetsuo Uchikoshi
    • Organizer
      The 7th International Conference on the Characterization and Control of Interfaces for High Quality Advanced Materials
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 制御されたナノ構造に基づく発光特性の強靱化と素子創製2021

    • Author(s)
      白幡直人
    • Organizer
      粉体粉末冶金協会2021年度秋季大会(第128回講演大会)
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] シェル成長を制御したInP/ZnSコア/シェル構造半導体量子ドットの狭い半値全幅フォトルミネッセンス2021

    • Author(s)
      根本一宏, 白幡直人
    • Organizer
      第72回コロイドおよび界面化学討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 鉛フリーハライドダブルペロブスカイトナノ結晶の合成と光学特性2021

    • Author(s)
      Xiaoyu Huang, 白幡直人
    • Organizer
      日本セラミックス協会第34回秋季シンポジウム
    • Related Report
      2021 Annual Research Report
  • [Presentation] 高輝度かつ発光波長可変なコロイダルシリコン量子ドット発光ダイオード2021

    • Author(s)
      山田博之, 白幡直人
    • Organizer
      日本セラミックス協会第34回秋季シンポジウム
    • Related Report
      2021 Annual Research Report
  • [Presentation] シリコン量子ドットを発光層に具備する近赤外発光ダイオードの作製と評価2021

    • Author(s)
      渡邊純平, 石井靖, 白幡直人
    • Organizer
      日本セラミックス協会第15回関西支部学術講演会
    • Related Report
      2021 Annual Research Report
  • [Book] System-Material Nanoarchitectonics2022

    • Author(s)
      Naoto Shirahata
    • Total Pages
      352
    • Publisher
      Springer
    • Related Report
      2022 Annual Research Report
  • [Remarks] SAMURAI

    • URL

      https://samurai.nims.go.jp/profiles/shirahata_naoto?locale=ja

    • Related Report
      2023 Annual Research Report 2022 Annual Research Report 2021 Annual Research Report
  • [Patent(Industrial Property Rights)] 量子ドットおよびその製造方法、緑色の蛍光体、可視化染料並びに顔料2021

    • Inventor(s)
      白幡直人、根本一宏
    • Industrial Property Rights Holder
      物質・材料研究機構
    • Industrial Property Rights Type
      特許
    • Filing Date
      2021
    • Related Report
      2021 Annual Research Report

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

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