Achieving High Thermoelectric Performance and Metallic Transport in Solvent‐Sheared PEDOT:PSS

Abstract Polymer‐based materials hold great potential for use in thermoelectric applications but are limited by their poor electrical properties. Through a combination of solution‐shearing deposition and directionally applied solvent treatments, poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) thin films with metallic‐like conductivities can be obtained with high power factors in excess of 800 µW m −1 K −2 . X‐ray scattering and absorption data indicate that structural alignment of PEDOT chains and larger‐sized domains are responsible for the enhanced electrical conductivity. It is expected that further enhancements to the power factor can be obtained through device geometry and postdeposition solvent shearing optimization.