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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]

Since the late '80s, a highly stable conductive polymer has been developed, that is poly(3,4-ethylene dioxythiophene), also known as PEDOT. Its increasing conductivity throughout the years combined with its intrinsic stability have aroused great attention both in the academic and industrial fields. The growing importance of PEDOT, can be easily acknowledged through the numerous applications in thermoelectricity, photovoltaics, lighting, sensing, technical coatings, transparent electrodes, bioelectronics, and so forth. Although its high electrical conductivity is strongly established in the literature, the wide range of data shows that disorder, as the limiting factor in charges' transport, hinders the design of materials with optimal performances. The aim of this article is to review and discuss recent progresses dealing with the electrical conductivity and transport properties in PEDOT materials, with special attention on morphological and structural features. Particular emphasis is given to the commercial PEDOT:PSS as well as other PEDOT-based materials stabilized with smaller counter-anions. It appears that the electrical conductivity and the transport mechanisms are closely related to the fabrication process, the crystallinity of the material and the choice of the counter-anions. With the tunable electrical properties, new functionalities appear accessible and add up to the already existing applications that are concisely highlighted. [ABSTRACT FROM AUTHOR]