Publication date: 15th December 2025
During the past decades, π-conjugated polymers (CPs) and oligomers have attracted extensive attentions on account of their peculiar optical properties, high conductivities and low-cost fabrication process. Poly(9,9-dioctylfluorene) (PFO) is a typical blue-emitting polymer capable of forming a β-phase conformation, which enhances conjugation length, chain packing, and the Förster radius for energy transfer. However, PFO suffers from photochemical instability and green-band emission under photo-oxidation. Here, Polydiarylfluorene-based conjugated polymers have emerged as versatile platforms for exploring the interplay between chain conformation, solid-state order, and photophysical gain processes. We present a unified investigation bridging structural evolution and optical amplification in these polymers. By combining calorimetry, grazing-incidence wide-angle X-ray scattering, and spectroscopic analyses, we reveal that thermally induced conformational ordering governs the emergence of emissive domains and the onset of amplified spontaneous emission. Complementary studies on phenyl-modified poly(diarylfluorene-co-N-phenyl) derivatives further demonstrate that controlled disruption of π–π stacking through chain twisting effectively suppresses exciton–exciton annihilation and enhances stimulated emission. These results highlight that both the establishment and modulation of conformational order are key to balancing exciton transport and gain stability in conjugated polymer films. Our findings provide fundamental insights into how molecular conformation dictates the photophysical pathways underlying light amplification in organic semiconductors, offering rational guidelines for the design of high-gain polymer emitters.
C.S. acknowledges Guangdong Basic and Applied Basic Research Foundation (Grant No. 2024A1515110084) and Guangdong Pearl River Talent Program (Grant No. 2023QN10Z748). We acknowledge the European Synchrotron Radiation Facility (ESRF) for the provision of beam time on the DUBBLE BM26 beamline and would like to thank Dr. Daniel Hermida for their assistance.
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