Tuning the physicochemical properties of conjugated polymers via intramolecular noncovalent interactions

• • NoCL incorporation increases polymer chain rigidity, as evidenced by temperature-dependent absorption spectroscopy showing suppressed non-radiative decay pathways; this directly enhances charge transport mobilities critical for OFET and OSC performance. • • Cryo-EM and freeze-drying TEM reveal that NoCLs promote the formation of pre-aggregates with optimal length, which correlates with improved intermolecular interactions and potentially higher fill factors in organic solar cells. • • DLS and SANS measurements confirm that NoCLs enhance intermolecular interactions in solution, leading to more ordered solid-state packing; this addresses the bottleneck of poor crystallinity in conjugated polymers. • • The combined theoretical and experimental approach establishes a quantitative link between NoCL strength (typically two orders of magnitude weaker than covalent bonds) and macroscopic transport properties, enabling predictive design of CPs with tailored physicochemical characteristics.