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The nature of chain aggregation in solution always results in variable spin-coated film mesoscale morphology and uncontrollable device performance. The abundant variety and increasing chemical complexity of conjugated polymers induced additional diverse electrostatic and dispersion interactions (non-covalent interactions), although it is not fully understood how the interplay of these forces results in the observed conformational order, chain aggregates and film morphologies. Herein, we present a precise study on the role of non-covalent interaction in the self-organization behavior, conformational order and optoelectrical properties of polyfluorene (PPFOH) toward tuning its electroluminescence (EL). The supramolecular PPFOH system consisted of an intrinsically doped hydrogen-bond-assisted microstructure as a “guest” and a blue light-emitting backbone chain as a “host”, which show a special binary emissive property of solution-induced self-dopant formation in the amorphous films. As a result of a strong non-covalent interaction between polymer chains and solvent molecules (type II solvent), a likely distorted or fold chain in rod-coil or branch cluster shows a narrow and strong aggregation emission at 525–540 nm. Low-polar solvents (called type I) can also induce a shoulder low-energy emission at 550–580 nm in the films, attributed to the extended and stretched chain complex for the tendency of interchain hydrogen-bonding interaction. Further evidence from nanoscale infrared (AFM-IR) analysis confirmed the stronger hydrogen-bonding interaction in the type II films than those in the type I films. Finally, supramolecular PPFOH electroluminescence colours can be tuned from blue to sky blue, green, white, yellow and orange. [ABSTRACT FROM AUTHOR]

Heteroatomic conjugated polymers (HCPs) can have complicated molecular structures with several heteroatoms in the repeat unit, which is helpful for designing color-tunable emitters, photovoltaic donors and high mobility materials. In order to understand their relatively complex molecular superstructure characteristics in depth, heteroatomic substitution-induced diverse non-covalent interactions must be investigated. Here, we systematically studied the gelation processing and its influence on the optoelectronic properties of a series of sp2 nitrogen (N) substituted polyfluorenes (PF8-co-DAF8) towards highly stable blue polymer light-emitting diodes (PLEDs). This heteroatomic substitution allows for diverse chain C–H…N hydrogen bonds, correlating with an excellent gelation behavior at room temperature. Films with a gelation superstructure show a weak interchain π–π interaction and energy transfer compared to non-gelation ones. PLEDs based on a gelation film give a stable, deep-blue emission with CIE coordinates of (0.16, 0.17) and a luminous efficiency (L.E.) of 1.30 cd A−1, while non-gelation film-based PLEDs display a stable, sky-blue emission (CIE: 0.20, 0.24; L.E.: 2.13 cd A−1). Diverse non-covalent interactions originating from the heteroatomic substitution cause a complicated molecular aggregation behavior in solution that can significantly affect the chain rearrangement in the film-casting process, thereby dominating the optoelectrical properties. [ABSTRACT FROM AUTHOR]