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Poly(3,4-ethylenedioxythiophene) (PEDOT) is certainly the most known and most used conductive polymer because it is commercially available and shows great potential for organic electronic, photovoltaic, and thermoelectric applications. Studies dedicated to PEDOT films have led to high conductivity enhancements. However, an exhaustive understanding of the mechanisms governing such enhancement is still lacking, hindered by the semicrystalline nature of the material itself. In this article, we report the development of highly conductive PEDOT films by controlling the crystallization of the PEDOT chains and by a subsequent dopant engineering approach using iron(III) trifluoromethanesulfonate as oxidant, N-methyl pyrrolidone as polymerization rate controller and sulfuric acid as dopant. XRD, HRTEM, Synchrotron GIWAXS analyses and conductivity measurements down to 3 K allowed us to unravel the organization, doping, and transport mechanism of these highly conductive PEDOT materials. N-methyl pyrrolidone promotes bigger crystallites and structure enhancement during polymerization, whereas sulfuric acid treatment allows the replacement of triflate anions by hydrogenosulfate and increases the charge carrier concentration. We finally propose a charge transport model that fully corroborates our experimental observations. These polymers exhibit conductivities up to 5400 S cm-1 and thus show great promise for room temperature thermoelectric applications or ITO alternative for transparent electrodes. [ABSTRACT FROM AUTHOR]

All-polymeric flexible transparent heaters (THs) are demonstrated for the first time. Thin films of four poly(3,4-ethylenedioxythiophene) (PEDOT)-based materials embedding different dopants exhibit low sheet resistances, down to 57 Ω sq -1 associated with good transparencies (>87%) and a haze lower than 1%. These transparent thin films show excellent heating properties, with high heating rates (up to 1.6 °C s -1 ) and steady-state temperatures exceeding 100 °C when subjected to 12 V bias. Very high areal power densities were also measured, reaching almost 10 000 W m -2 . The temperature increase is finely fitted to a thermal model. It is further demonstrated that these new THs can be efficiently integrated for applications in thermochromic displays and visor deicers.