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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]

Poly(3,4-ethylenedioxythiophene) (PEDOT) is a transparent conductive polymer widely used in flexible photonic and optoelectronic devices because of its excellent electrical and optical properties. However, its current range of applications is limited by its poor stability under high humidity and solar radiations. Encapsulation is an attractive solution to this problem and the development of a low-temperature and scalable deposition method is highly desirable. In this study, we report the use of spatial atomic layer deposition (SALD) to deposit ultrathin layers of ZnO, TiO 2 , and Al 2 O 3. These nanolayers maintain the electrical performance of the conductive polymer and its high optical transmittance. The use of SALD ensures low-cost and flexible processing with pinhole-free high-quality coatings at atmospheric pressure and high-throughput. The present study is the first to investigate the effect of various multilayer metal oxide encapsulations on the long-term stability of PEDOT-based transparent conductive materials under solar radiations. We demonstrate finally that bilayer TiO 2 /Al 2 O 3 and TiO 2 /ZnO coatings preserve the optoelectronic properties of three different PEDOT-based films, namely PEDOT:OTf (OTf = triflate), PEDOT:Sulf (Sulf = sulfate)and PEDOT:PSS (PSS = PolyStyreneSulfonate) films. [Display omitted] • PEDOT materials are encapsulated using spatial atomic layer deposition. • Deposition of nanolayers is an efficient method to preserve the electrical performances of highly conductive PEDOT. • Bilayer structures TiO 2 /ZnO and TiO 2 /Al 2 O 3 lead to the most effective protection. [ABSTRACT FROM AUTHOR]