Fluorene Oligomers Featuring a Central 2,1,3-Benzothiadiazole Unit with High Photoluminescence Quantum Yield and Amplified Spontaneous Emission

IF 5.1 1区化学 Q1 POLYMER SCIENCE

Macromolecules Pub Date : 2025-03-02 DOI:10.1021/acs.macromol.4c03110

Philipp J. Welscher, Ulrich Ziener, Alexander J. C. Kuehne

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Abstract

Fluorene-based conjugated materials are pivotal to optoelectronic applications due to their tunable optical properties and high photoluminescence quantum yields. While conjugated polymers like poly(fluorene-co-benzothiadiazole) have been extensively studied, their performance is often limited by product inhomogeneity and morphological constraints. Oligofluorenes, with their well-defined structures and controlled morphologies, offer a promising alternative but have been underexplored in substoichiometric fluorene-benzothiadiazole systems. Here, we report the synthesis and characterization of a novel series of substoichiometric fluorene-BT oligomers featuring a central BT unit flanked by dioctylfluorene arms of varying repeat lengths, ranging from trimers to heptamers. These oligomers exhibit superior optical properties compared to conventional F8BT polymers, including enhanced quantum yields and amplified spontaneous emission thresholds of down to 1.5 μJ cm^–2. The optical performance is analyzed in relation to oligomer length and fluorene-to-BT ratio, providing insights into the relationship between molecular design and photophysical behavior. Our findings highlight the potential of these defect-free, tunable green-emitting oligomers for next-generation light-emitting diodes and low-threshold lasers, paving the way for further advancements in photonic and optoelectronic materials.

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芴基共轭材料具有可调光学特性和高光致发光量子产率，因此在光电应用中举足轻重。虽然人们已经对聚（芴-共苯并噻二唑）等共轭聚合物进行了广泛研究，但它们的性能往往受限于产品的不均匀性和形态限制。低聚芴具有定义明确的结构和可控的形态，是一种很有前景的替代品，但在亚计量芴-苯并噻二唑体系中的研究还很不够。在此，我们报告了一系列新型亚计量芴-苯并噻二唑低聚物的合成和表征，这些低聚物具有一个中心苯并噻二唑单元，两侧是重复长度各异的二辛基芴臂，从三聚体到七聚体不等。与传统的 F8BT 聚合物相比，这些低聚物具有更优越的光学性能，包括量子产率提高，自发辐射阈值放大到 1.5 μJ cm-2。我们分析了光学性能与低聚物长度和芴-BT 比率的关系，从而深入了解了分子设计与光物理行为之间的关系。我们的研究结果凸显了这些无缺陷、可调谐的绿色发光低聚物在下一代发光二极管和低阈值激光器中的应用潜力，为光子和光电材料的进一步发展铺平了道路。

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来源期刊

Macromolecules 工程技术-高分子科学

CiteScore

9.30

自引率

16.40%

发文量

942

审稿时长

2 months

期刊介绍： Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.