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Item type:Publication, Access status: with files , Strategies for optimizing hydrophobic semiconducting polymers for OECTs: modifications and additives(2026); Organic electrochemical transistors (OECTs) are promising for bioelectronics and neuromorphic computing but face challenges with organic mixed ion-electron conductors (OMIECs), such as swelling and limited synthesis flexibility. This research explores the synthesis of organometallics ruthenium (Ru)-containing polymetallaynes and engineering established hydrophobic organic semiconducting polymers (OSCPs). Ru-polymetallaynes were modified with different ligands to introduce ligand planarity and redox matching, where dithienopyrrole (DTP) showed the best performance due to enhanced metal-metal (M-M) interactions as a result of redox-matching, exhibiting enhanced state-retention ability and making it suitable for non-volatile memory applications. To improve OSCPs’ OECT performance, two metal-containing additives were investigated: poly(vinylferrocene) (PVF+) improved P3HT doping efficiency and device response time via enhanced hydrophilicity in the PVF+/P3HT blends, while poly(ethylene glycol) functionalized gold nanoparticles (PEG-AuNPs)/P3HT composites showed increased charge mobility (µ) and volumetric capacitance (C*), significantly improving OMIEC metrics such as µC*, making the OSCPs comparable to state-of-the-art OMIECs. Overall, incorporating metal-containing additives into hydrophobic OSCPs enhances both electronic and ionic performance, expanding the potential applications of this class of materials in OECTs.Publicationtype: Doctoral Thesis46 21