Recent advancements in the field of organic electronics and bioelectronics have focused on the processing of PEDOT:PSS with ionic additives to promote high electrical conductivity and device performance. The combination of excellent electrical properties and tunable structure are increasingly attractive, however, the mechanism responsible for these properties, specifically from a solution-phase self-assembly perspective, is unknown. Herein, we reveal how solution-phase self-assembly of PEDOT:PSS with ionic additives leads to multiscale ordering which influences thin film microstructure, electronic properties, enables new additive manufacturing modalities, and applications in aqueous environments.
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