“…Whether in lightweight organic photovoltaics, − flexible organic light-emitting diodes, − organic sensors, − organic field-effect transistors, − transparent organic electrodes, − or organic thin-film thermoelectrics, − nowadays, organic semiconductors play a fundamental part in the development of new trendsetting devices and applications. The reason for this lies in the advantageous properties of organic semiconductors, like their easy and low-temperature processability from solution, facilitating a low-cost and energy-efficient fabrication with large-scale deposition techniques like printing, spray, or dip coating. , Furthermore, the raw materials are usually abundantly available and enable low or nontoxic, lightweight, and mechanical flexible devices. Besides organic small molecules, like oligothiophene, fullerene, perylene, or anthracene derivatives, an intense research interest lies in polymer-based organic semiconductors, usually based on polyacetylene, polypyrrole, polyphenylene vinylene, or polythiophene backbones. − In particular, great attention is paid to the blend poly(3,4-ethylene dioxythiophene):polystyrene sulfonate (PEDOT:PSS), which comprises the insoluble, however, excellent p-type semiconductor PEDOT and PSS, a water-soluble partly negatively charged polyanion. , Besides the before mentioned advantages of organic semiconductors, PEDOT:PSS also exhibits a tunable and potentially high hole conductivity of up to 10 3 S cm –1 , which even competes with commonly used transparent electrode materials like indium tin oxide (ITO). − The key to the easy tunability of optoelectronic properties lies in the particular polymer blend morphology of PEDOT:PSS. ,, In an aqueous solution, the insoluble π-conjugated PEDOT chains agglomerate, forming a PEDOT enriched core, which is surrounded and stabilized by a shell of water-soluble PSS.…”