Publication date: 21st July 2025
Organic electrochemical transistors operate via electrochemical doping, where an applied gate potential in an electrolyte modulates the channel conductivity through counterion injection into and expulsion from the semiconducting polymer. This process, and the resulting current in devices, affects and is affected by the structure of the underlying organic mixed ionic-electronic conductor (OMIEC) and the polymer-electrolyte interface, ultimately impacting a range of properties including doping/dedoping kinetics, polymer mechanics, charge transport, and doping efficiency. Given the nanostructured nature of OMIECs, scanning probe microscopy techniques can reveal important information about the underlying process, particularly as these methods can be performed operando in aqueous electrolytes. Here we discuss microscopy-driven investigations using optical and atomic force microscopy methods to probe the OMIECs before, during, and after the electrochemical doping process. We use these methods to explore tradeoffs between sidechain chemistry and uptake, as well as how elastic modulus and adhesion change upon oxidation. Beyond mechanics, we discuss how materials can exhibit vastly different levels of doping efficiency, using a combination of Kelvin probe force microscopy and spectroelectrochemistry to provide insight into charge transport models and delocalized carrier density. Together, these methods link real-space operando measurements with device level performance and can provide a rational basis for optimizing materials.
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