Thermodynamics of organic electrochemical transistors

Matteo Cucchi (), Anton Weissbach, Lukas M. Bongartz, Richard Kantelberg, Hsin Tseng, Hans Kleemann and Karl Leo
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Matteo Cucchi: Neuro-X Institute, École Polytechnique Fédérale de Lausanne (EPFL)
Anton Weissbach: Technische Universität Dresden
Lukas M. Bongartz: Technische Universität Dresden
Richard Kantelberg: Technische Universität Dresden
Hsin Tseng: Technische Universität Dresden
Hans Kleemann: Technische Universität Dresden
Karl Leo: Technische Universität Dresden

Nature Communications, 2022, vol. 13, issue 1, 1-8

Abstract: Abstract Despite their increasing usefulness in a wide variety of applications, organic electrochemical transistors still lack a comprehensive and unifying physical framework able to describe the current-voltage characteristics and the polymer/electrolyte interactions simultaneously. Building upon thermodynamic axioms, we present a quantitative analysis of the operation of organic electrochemical transistors. We reveal that the entropy of mixing is the main driving force behind the redox mechanism that rules the transfer properties of such devices in electrolytic environments. In the light of these findings, we show that traditional models used for organic electrochemical transistors, based on the theory of field-effect transistors, fall short as they treat the active material as a simple capacitor while ignoring the material properties and energetic interactions. Finally, by analyzing a large spectrum of solvents and device regimes, we quantify the entropic and enthalpic contributions and put forward an approach for targeted material design and device applications.

Date: 2022
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DOI: 10.1038/s41467-022-32182-7

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