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  1. The conductivity and charge transport mobility of conjugated polymers (CPs) are largely correlated with their degree of crystallinity, rendering the crystallization of CPs an important endeavour. However, such tasks can be challenging, especially in the absence of sidechain functionalization. In this study, we demonstrate that the incorporation of a small amount of oligomers, specifically tetraaniline, can induce crystallization of the parent polymer, polyaniline, through a single-step self-assembly process. The resulting crystals are compositionally homogeneous because the oligomers and their parent polymer share the same repeating unit and are both electroactive. Mechanistic studies reveal that the tetraaniline forms a crystalline seed that subsequently guides the assembly of polyaniline due to their structural similarities. Applying this oligomer-assisted crystallization approach to polyaniline with defined molecular weights resulted in single crystalline nanowires for 5000 Da polyaniline, and nanowires with strong preferential chain orientation for those with molecular weights between 10 000 and 100 000 Da. Absorption studies reveal that the polymer chains are in an expanded conformation, which likely contributed to the high degree of packing order. Two-probe, single nanowire measurements show that the crystals have conductivity as high as 19.5 S cm −1 . This method is simple, general, and can potentially be applied to other CPs. 
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  2. Conducting polymer hydrogels combine electrical conductivity and tunable water content, rendering them strong candidates for a range of applications including biosensors, cell culture platforms, and energy storage devices. However, these hydrogels are mechanically brittle and prone to damage, prohibiting their use in emerging applications involving dynamic movement and large mechanical deformation. Here, we demonstrate that applying the concept of architecture to conducting polymer hydrogels can circumvent these impediments. A stereolithography 3D printing method is developed to successfully fabricate such hydrogels in complex lattice structures. The resulting hydrogels exhibit elastic compressibility, high fracture strain, enhanced cycling stability, and damage-tolerant properties despite their chemical composition being identical to their brittle, solid counterparts. Furthermore, concentrating the deformation to the 3D geometry, rather than polymer microstructure, effectively decouples the mechanical and electrical properties of the hydrogel lattices from their intrinsic properties associated with their chemical composition. The confluence of these new physical properties for conducting polymer hydrogels opens broad opportunities for a myriad of dynamic applications. 
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  3. Abstract

    Materials are more easily damaged during accidents that involve rapid deformation. Here, a design strategy is described for electronic materials comprised of conducting polymers that defies this orthodox property, making their extensibility and toughness dynamically adaptive to deformation rates. This counterintuitive property is achieved through a morphology of interconnected nanoscopic core–shell micelles, where the chemical interactions are stronger within the shells than the cores. As a result, the interlinked shells retain material integrity under strain, while the rate of dissociation of the cores controls the extent of micelle elongation, which is a process that adapts to deformation rates. A prototype based on polyaniline shows a 7.5‐fold increase in ultimate elongation and a 163‐fold increase in toughness when deformed at increasing rates from 2.5 to 10 000% min−1. This concept can be generalized to other conducting polymers and highly conductive composites to create “self‐protective” soft electronic materials with enhanced durability under dynamic movement or deformation.

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