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Development and mechanism elucidation of thermostable transparent room temperature phosphorescent polymers based on high pressure-induced change in emission spectrum

Research Project

Project/Area Number 21H01995
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 35020:Polymer materials-related
Research InstitutionTokyo Institute of Technology

Principal Investigator

ANDO SHINJI  東京工業大学, 物質理工学院, 教授 (00272667)

Co-Investigator(Kenkyū-buntansha) 石毛 亮平  東京工業大学, 物質理工学院, 准教授 (20625264)
Project Period (FY) 2021-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥13,260,000 (Direct Cost: ¥10,200,000、Indirect Cost: ¥3,060,000)
Fiscal Year 2023: ¥1,950,000 (Direct Cost: ¥1,500,000、Indirect Cost: ¥450,000)
Fiscal Year 2022: ¥4,290,000 (Direct Cost: ¥3,300,000、Indirect Cost: ¥990,000)
Fiscal Year 2021: ¥7,020,000 (Direct Cost: ¥5,400,000、Indirect Cost: ¥1,620,000)
Keywords高圧誘起発光 / ダイアモンド・アンビル・セル / 顕微分光 / 時間依存密度汎関数法 / 高発光性ポリイミド / 連続照射誘起遅延発光 / 室温燐光 / 酸素消光 / ダイヤモンド・アンビル・セル
Outline of Research at the Start

室温長寿命燐光を示す発光性ポリマーとそのモデル化合物に対して,高圧(~10万気圧)と低温(-196℃~)を印加しつつ,励起・発光スペクトル,量子収率,発光寿命を測定するともに,赤外・Ramanスペクトル,広角X線回折の観測により,高圧下での発光強度増大の原因を解明する.高圧下では体積圧縮により高分子の局所振動が抑制され,コンホメーションや凝集状態変化が生じるため,振動緩和や項間交差に大きな摂動がかかり、励起状態の光物理過程が変化する.その知見に量子化学計算を合わせ,無色透明性を維持しつつ,室温長寿命燐光や大きな圧力誘起発光増強性を示す新規耐熱性芳香族ポリマー群を創製し,実用化検討に発展させる.

Outline of Final Research Achievements

There are two notable achievements of this research project. First, we found that thin films of three imide compounds dispersed in a transparent matrix (PMMA) exhibit extremely long-lived green phosphorescence (more than a few seconds) as well as blue fluorescence emission at room temperature in air. After an "induction time" of several minutes, the phosphorescent emission gradually increases and approaches saturation, and a dark green afterglow of several seconds or more is emitted after the end of irradiation. Second, room-temperature phosphorescence of different imide compounds and polyimides containing bromine atoms showed a remarkable enhancement of luminescence intensity when ultrahigh pressure was applied (1-8.5 GPa). This phenomenon is known as pressure-induced emission enhancement (PIEE) and is the first observation of PIEE in room-temperature phosphorescence emitted by an amorphous polymer (polyimide).

Academic Significance and Societal Importance of the Research Achievements

室温常圧での遅延燐光発光はこれまでも知られていたが,長時間照射遅延燐光(PIDL)においては,酸素存在下では燐光の発光開始までに明確な誘導時間が存在すること,真空中では誘導時間が観測されないこと,誘導時間は雰囲気中の酸素濃度に比例すること,そして燐光寿命が照射時間にともなって増強される蓄光性を示すことが新たな発見であり,高解像ナノイメージングや高感度センシングに応用可能である.また,超高圧印加による圧力誘起発光増強現象も知られていたが,対象は有機低分子結晶に限られており,高耐熱性を有する非晶性ポリイミドにおいて観測されたことは新たな発見であり,極端条件下での圧力センサーなどに応用可能である.

Report

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

    (38 results)

All 2024 2023 2022 2021 Other

All Int'l Joint Research (5 results) Journal Article (15 results) (of which Int'l Joint Research: 3 results,  Peer Reviewed: 15 results,  Open Access: 6 results) Presentation (17 results) (of which Int'l Joint Research: 10 results,  Invited: 4 results) Remarks (1 results)

  • [Int'l Joint Research] ヴィルニュス物理科学研究所(リトアニア)

    • Related Report
      2023 Annual Research Report
  • [Int'l Joint Research] 中国科学院過程工程研究所(中国)

    • Related Report
      2023 Annual Research Report
  • [Int'l Joint Research] コンスタンツ大学(ドイツ)

    • Related Report
      2023 Annual Research Report
  • [Int'l Joint Research] ビルニュス物理科学研究所(リトアニア)

    • Related Report
      2022 Annual Research Report
  • [Int'l Joint Research] ビルニュス物理科学研究所(リトアニア)

    • Related Report
      2021 Annual Research Report
  • [Journal Article] Polarization Analysis and Humidity Dependence of Dielectric Properties of Aromatic and Semialicyclic Polyimides Measured at 10 GHz2024

    • Author(s)
      Ririka SAWADA, Shinji ANDO
    • Journal Title

      J. Phys. Chem. C

      Volume: 128 Issue: 16 Pages: 6979-6990

    • DOI

      10.1021/acs.jpcc.4c01201

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Photophysical Analysis of Dual Fluorescence and Phosphorescence Emissions Observed for Semi-Aliphatic Polyimides at Lower Temperatures2024

    • Author(s)
      Mayuko NARA, Eisuke FUJIWARA, Aurimas VYSNIAUSKAS, Vidmantas GULBINAS, Shinji ANDO
    • Journal Title

      Phys.Chem.Chem.Phys.

      Volume: 26 Issue: 21 Pages: 15461-15471

    • DOI

      10.1039/d4cp00538d

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Characteristic Changes in the Structures and Properties of Polyimides Induced by Very High Pressure up to 8 GPa2023

    • Author(s)
      Shinji ANDO
    • Journal Title

      Polymer Journal (Focus review)

      Volume: 55 Issue: 6 Pages: 645-652

    • DOI

      10.1038/s41428-023-00759-8

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Troeger's Base (TB)-Based Polyimides as Promising Heat-Insulating and Low-K Dielectric Materials2023

    • Author(s)
      Jian LU, Yu ZHANG, Jing LI, Meifang FU, Guoxiang ZOU, Shinji ANDO, Yongbing ZHUANG
    • Journal Title

      ACS Macromolecules

      Volume: 56 Issue: 5 Pages: 2164-2174

    • DOI

      10.1021/acs.macromol.2c02148

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Vertically Aligned Polyimide Films Prepared from Lyotropic Liquid-crystalline Smectic Precursors2023

    • Author(s)
      Shohei HARA, Shinji ANDO, Ryohei ISHIGE
    • Journal Title

      Polymer

      Volume: 281 Pages: 126100-126100

    • DOI

      10.1016/j.polymer.2023.126100

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Enhancing Optical, Dielectric, and Thermal Properties of Bio-based Polyimides Incorporating Isomannide with a Bent and Sterically Constrained Conformation2023

    • Author(s)
      Ririka SAWADA, Shinji ANDO
    • Journal Title

      J. Mater. Chem. C

      Volume: 11 Issue: 43 Pages: 15053-15053

    • DOI

      10.1039/d3tc02933f

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Large-Stokes-shifted Yellow Photoluminescence Emission from an Imide and Polyimides Forming Multiple Intramolecular Hydrogen Bonds2022

    • Author(s)
      Naiqiang LIANG, Shigeki KUWATA, Ryohei ISHIGE, Shinji ANDO
    • Journal Title

      Mater. Chem. Front

      Volume: 5 Issue: 1 Pages: 24-32

    • DOI

      10.1039/d1qm01280k

    • Related Report
      2023 Annual Research Report 2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Colorless, Low Dielectric, and Optically Active Semialicyclic Polyimides Incorporating a Biobased Isosorbide Moiety in the Main Chain2022

    • Author(s)
      Ririka SAWADA, Shinji ANDO
    • Journal Title

      Macromolecules

      Volume: 55 Issue: 15 Pages: 6787-6800

    • DOI

      10.1021/acs.macromol.2c01288

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Photoluminescence Properties of Copolyimides Containing Naphthalene Core and Analysis of Excitation Energy Transfer between the Dianhydride Moieties2021

    • Author(s)
      Marina DOI, Koichiro MUTO, Mayuko NARA, Naiqiang LIANG, Kosuke SANO, Hiroaki MORI, Ryohei ISHIGE, Shinji ANDO
    • Journal Title

      Journal of Photopolymer Science and Technology

      Volume: 34 Issue: 5 Pages: 423-430

    • DOI

      10.2494/photopolymer.34.423

    • NAID

      130008119626

    • ISSN
      0914-9244, 1349-6336
    • Year and Date
      2021-06-11
    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Quantitative analysis of stereoscopic molecular orientations in thermally reactive and heterogeneous noncrystalline thin films via variable-temperature infrared pMAIRS and GI-XRD2021

    • Author(s)
      Ishige Ryohei、Tanaka Kazuyuki、Ando Shinji
    • Journal Title

      Polymer Journal

      Volume: 53 Issue: 5 Pages: 603-617

    • DOI

      10.1038/s41428-020-00458-8

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Ultrafast-Spectroscopic Analysis of Pressure-Induced Variations of Excited-State Energy and Intramolecular Proton Transfer in Semi-Aliphatic Polyimide Films2021

    • Author(s)
      Eisuke FUJIWARA, Ryoji ORITA, Aurimas VYSNIAUSKAS, Marius FRANCKEVICIUS, Ryohei ISHIGE, Vidmantas GULBINAS, Shinji ANDO
    • Journal Title

      J. Phys. Chem. B. (ACS)

      Volume: 125 Issue: 9 Pages: 2425-2434

    • DOI

      10.1021/acs.jpcb.0c11500

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Full-Colour Solvatochromic Fluorescence Emitted from a Semi-Aromatic Imide Compound Based on ESIPT and Anion Formation2021

    • Author(s)
      Atsuko TABUCHI, Teruaki HAYAKAWA, Shigeki KUWATA, Ryohei ISHIGE, Shinji ANDO
    • Journal Title

      Mater. Adv. (RSC)

      Volume: 5 Issue: 17 Pages: 5629-5638

    • DOI

      10.1039/d1ma00308a

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Colorless Copolyimide Films Exhibiting Large Stokes-Shifted Photoluminescence Applicable for Spectral Conversion2021

    • Author(s)
      Naiqiang LIANG, Eisuke FUJIWARA, Mayuko NARA, Ryohei ISHIGE, Shinji ANDO
    • Journal Title

      ACS Appl. Polym. Mater.

      Volume: 3 Issue: 8 Pages: 3911-3921

    • DOI

      10.1021/acsapm.1c00474

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Compression and Thermal Expansion Behaviors of Highly Crystalline Polyimide Particles Prepared from Poly(amic acid) and Monomer Salts2021

    • Author(s)
      Eisuke FUJIWARA, Ryohei ISHIGE, D. Alonso CERRON-INFANTES, M. Josef TAUBLAENDER, Miriam M. UNTERLASS, Shinji ANDO
    • Journal Title

      Macromolecules

      Volume: 54 Issue: 18 Pages: 8714-8725

    • DOI

      10.1021/acs.macromol.1c00779

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Synthesis and Characterization of White-Light Luminescent End-Capped Polyimides Based on FRET and Excited State In-tramolecular Proton Transfer2021

    • Author(s)
      Atsuko TABUCHI, Teruaki HAYAKAWA, Shigeki KUWATA, Ryohei ISHIGE, Shinji ANDO
    • Journal Title

      Polymers (MDPI)

      Volume: 13 Issue: 22 Pages: 4050-4050

    • DOI

      10.3390/polym13224050

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access
  • [Presentation] Large-Stokes-shifted Dual Photoluminescence of Thianthrene-containing Imide Compounds and Polyimides Undergoing Transient Conformational Changes2024

    • Author(s)
      Shinji ANDO, Hiroka YAMAMATSU
    • Organizer
      Polycondensation 2024 (Lyon, France)
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Optical Properties of Thiol-containing Imide Compound via Excited State Intramolecular Proton Transfer2024

    • Author(s)
      Yuka ANDO, Marina DOI, Atsuko TABUCHI, Haonan LIU, Shinji ANDO
    • Organizer
      Polycondensation 2024 (Lyon, France)
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Polarization Analysis and Humidity Dependence of Dielectric Properties of Aromatic/Semi-Aromatic Polyimides at 10 GHz2024

    • Author(s)
      Ririka SAWADA, Haonan LIU, Shinji ANDO
    • Organizer
      Polycondensation 2024 (Lyon, France)
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Dielectric Properties of Various Polyimides in the mmWave Range2024

    • Author(s)
      Haonan LIU, Ririka SAWADA, Shana YANAGIMOTO, Yoshiyuki YANAGIMOTO, Shinji ANDO
    • Organizer
      Polycondensation 2024 (Lyon, France)
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Photophysical Processes and Sensor Properties of a Multicolor Fluorescent Polyimide with ESIPT Ability2023

    • Author(s)
      Shinji ANDO, Atsuko TABUCHI, Teruaki HAYAKAWA, Shigeki KUWATA, Ryohei ISHIGE,
    • Organizer
      STEPI-12 (Montpellier, France)
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Relationships between Molecular Structure and Optical, Dielectric, and Thermal Properties of Novel Semi-alicyclic Polyimides Containing Bio-derived Isohexides2023

    • Author(s)
      Ririka SAWADA, Mitsutaka OZAKI, Kazuhisa YAJIMA, Shinji ANDO
    • Organizer
      STEPI-12 (Montpellier, France)
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Analysis of Prolonged Irradiation-induced Delayed Luminescence of Imide Compounds Dispersed in Polymer Matrix2023

    • Author(s)
      Marina DOI, Ryohei ISHIGE, Shinji ANDO
    • Organizer
      STEPI-12 (Montpellier, France)
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Analysis and Applications of Anisotropic Structure and Properties of Polyimides Generated under Extreme Conditions (Plenary Lecture)2022

    • Author(s)
      Shinji ANDO
    • Organizer
      Polycondensation 2022 (Seoul, Korea)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Photophysical Mechanism of Prolonged Irradiation-induced Delayed Luminescence of Imide Compounds Dispersed in Polymer Matrices2022

    • Author(s)
      Marina DOI, Ryohei ISHIGE, Shinji ANDO
    • Organizer
      Polycondensation 2022 (Seoul, Korea)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Pressure-Induced Enhancement of Phosphoresce from Bromine-Containing Imide Compound and Polyimide2022

    • Author(s)
      Ryuichi ISODA, Koichiro MUTO, Marina DOI, Ryohei ISHIGE, Shinji ANDO
    • Organizer
      Polycondensation 2022 (Seoul, Korea)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] イミド化合物分散薄膜の紫外線連続照射により誘起される特異な遅延発光の生成機構2022

    • Author(s)
      土井 真里奈・石毛 亮平・安藤 慎治
    • Organizer
      高分子学会予稿集
    • Related Report
      2022 Annual Research Report
  • [Presentation] 燐光発光を示す含臭素イミド化合物およびポリイミドの圧力誘起発光増強現象の解明2022

    • Author(s)
      礒田 隆一・武藤 江一朗・土井 真里奈・石毛 亮平・安藤 慎治
    • Organizer
      高分子学会予稿集
    • Related Report
      2022 Annual Research Report
  • [Presentation] ナフタレンおよびビフェニル骨格を有する発光性イミド化合物の遅延発光特性2021

    • Author(s)
      土井 真里奈・武藤 江一朗・奈良 麻優子・梁 乃強・石毛 亮平・安藤 慎治・佐野 浩介・森 浩章
    • Organizer
      高分子学会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 燐光性含臭素ポリイミドの高圧印加による凝集状態と発光特性変化の相関解析2021

    • Author(s)
      礒田 隆一・武藤 江一朗・土井 真里奈・石毛 亮平・安藤 慎治
    • Organizer
      高分子学会
    • Related Report
      2021 Annual Research Report
  • [Presentation] ナフタレン,ビフェニルおよびオキシジフタル酸骨格を有する発光性イミド化合物の遅延発光特性2021

    • Author(s)
      士井 真里奈・武藤 江一朗・奈良 麻優子・梁 乃強・森 浩章・石毛 亮平・安藤 慎治
    • Organizer
      光化学若手の会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 高圧・高温下における耐熱性高分子の異方的な構造・物性変化の観測と機能開拓2021

    • Author(s)
      安藤 慎治
    • Organizer
      高分子学会予稿集
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] アダマンチル基を主鎖骨格に有する含硫黄ポリイミドの蛍光・燐光特性2021

    • Author(s)
      山松 寛華・田淵 敦子・梁 乃強・石毛 亮平・安藤 慎治
    • Organizer
      光化学討論会
    • Related Report
      2021 Annual Research Report
  • [Remarks] 東京工業大学物質理工学院 安藤研究室

    • URL

      http://www.ando-cap.mac.titech.ac.jp/

    • Related Report
      2023 Annual Research Report 2022 Annual Research Report 2021 Annual Research Report

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

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