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Quantifying the Three-Dimensional Molecular Arrangement in Polymer–Polymer Blends: Impact of Molecular Weight

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    Quantifying the Three-Dimensional Molecular Arrangement in Polymer–Polymer Blends: Impact of Molecular Weight
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    • Fei Dou
      Fei Dou
      School of Physics and Optoelectronic Engineering, Beijing Key Laboratory of Microstructure and properties of Solids, Beijing University of Technology, Institute of Information Photonic Technology, Beijing 100124, P. R. China
      Dept Mat, Imperial Coll London, Exhibit Rd, London SW7 2AZ, England
      Ctr Plast Elect, Imperial Coll London, Exhibit Rd, London SW7 2AZ, England
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      Orcidhttps://orcid.org/0000-0002-3867-6028
    • Yongli Ren
      Yongli Ren
      School of Physics and Optoelectronic Engineering, Beijing Key Laboratory of Microstructure and properties of Solids, Beijing University of Technology, Institute of Information Photonic Technology, Beijing 100124, P. R. China
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    • Liyang Yu
      Liyang Yu
      Research Institute of Frontier Science, Southwest Jiaotong University, Chengdu, Sichuan 610031, P. R. China
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    • Bo Xu
      Bo Xu
      Beijing Information Science and Technology University, Beijing 100192, P. R. China
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    • Matthew Dyson
      Matthew Dyson
      Eindhoven Univ Technol, Mol Mat & Nanosyst, Inst Complex Mol Syst, POB 513, Eindhoven NL-5600 MB, Netherlands
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      Orcidhttps://orcid.org/0000-0002-4502-6250
    • Jaime Martin
      Jaime Martin
      Univ Basque Country, POLYMAT, UPV EHU Ave Tolosa 72, San Sebastian 20018, Spain
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    • Zhuping Fei
      Zhuping Fei
      Institute of Molecular Plus, Department of Chemistry, Tianjin Key Laboratory of Molecular Optoelectronic Science, Tianjin University, Tianjin 300072, P. R. China
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      Orcidhttps://orcid.org/0000-0002-2160-9136
    • James H. Bannock
      James H. Bannock
      Dept Chem, Imperial Coll London, London W12 0BZ, England
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    • Yiwei Zhang
      Yiwei Zhang
      School of Physics and Optoelectronic Engineering, Beijing Key Laboratory of Microstructure and properties of Solids, Beijing University of Technology, Institute of Information Photonic Technology, Beijing 100124, P. R. China
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      Orcidhttps://orcid.org/0000-0001-5151-6419
    • Paul N. Stavrinou
      Paul N. Stavrinou
      Department of Engineering Science, University of Oxford, Parks Rd, Oxford OX1 3PJ, U.K.
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      Orcidhttps://orcid.org/0000-0001-6075-2587
    • Martin Heeney
      Martin Heeney
      Division of Physical Sciences & Engineering, King Abdullah University of Science and Technology, Thuwal, Jeddah 23955-6900, Kingdom of Saudi Arabia
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      Orcidhttps://orcid.org/0000-0001-6879-5020
    • John de Mello
      John de Mello
      Norwegian University of Science and Technology, Chemistry Høgskoleringen 5, Realfagbygget, Trondheim, NO-7491, Norsk
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      Orcidhttps://orcid.org/0000-0002-1704-2392
    • Xinping Zhang*
      Xinping Zhang
      School of Physics and Optoelectronic Engineering, Beijing Key Laboratory of Microstructure and properties of Solids, Beijing University of Technology, Institute of Information Photonic Technology, Beijing 100124, P. R. China
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0001-6534-0004
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    ACS Applied Polymer Materials

    Cite this: ACS Appl. Polym. Mater. 2025, 7, 5, 2986–2996
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsapm.4c03580
    Published March 1, 2025
    Copyright © 2025 American Chemical Society
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    Abstract

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    Solution-processed plastic semiconductors have garnered significant attention recently due to their ease fabrication and diverse optoelectronic functionalities, positioning them as promising contenders for the next generation of semiconductors. However, comprehending the molecular ordering in polymer semiconductor blends during solution processing remains a captivating challenge. In this study, we chose poly(3-hexylthiophene-2,5-diyl) (P3HT) and poly(3-hexylselenophene-2,5-diyl) (P3HS) blends as the model system and examined the molecular ordering of blends with low molecular weights (below the entanglement) and high molecular weights (above the entanglement). By employing a combination of structural analysis, spectroscopic techniques, and theoretical modeling, valuable insight regarding the arrangement of molecules in three dimensions within P3HT/P3HS blends of varying molecular weights have been acquired. Through these analyses, we establish a comprehensive relationship between molecular weight, molecular ordering, and exciton coherence in polymer–polymer blends.

    Copyright © 2025 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsapm.4c03580.

    • GPC curves for all the materials (Figure S1); differential scanning calorimetry (DSC) characterization of the solution cast neat films (Figure S2); DSC characterization of the solution cast blends (Figure S3); PL spectra and quadrature-PL spectra of P3HT:P3HS blends at 10 K (Figure S4); PL spectra and quadrature-PL spectra of P3HT and P3HS blends neat films at 10 and 300 K (Figure S5); PL spectra and quadrature-PL spectra of P3HT:P3HS blends at 300 K (Figure S6); temperature-dependent quadrature-PL spectra of the L/L blend (Figure S7); simulation parameters of neat polymers (Table S1); simulation parameters of blends (Table S2). quantified contribution of Quadrature PL to overall emission (Table S3) (PDF)

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    ACS Applied Polymer Materials

    Cite this: ACS Appl. Polym. Mater. 2025, 7, 5, 2986–2996
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsapm.4c03580
    Published March 1, 2025
    Copyright © 2025 American Chemical Society
    Request reuse permissions

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