As the bioelectronics field developed rapidly, organic electrochemical transistors (OECTs) are emerging as the “mainstay” of contemporary sensing platforms owing to their high-fidelity transduction of biological signals into electrical outputs. An underlying concept unveiling the working principle of OECTs is the implementation of the organic mixed ionic-electronic conductors (OMIECs), a subset of conjugated polymer, that can enable dual conduction pathways in ions/water and ionic-electronic coupling. In this respect, multiple advantages render OECTs the ideal devices for both sensing and amplifying biological signals in a wearable, low-operating voltages and high-transconductance fashion. However, a prominent barrier to OECT application is the lack of fundamental understanding of structure-property relationships, as there are very few high-performance OMIECs and the challenges and complications of in-situ/operando structural characterizations.<br/>Many state-of-the-art OMIECs come with intrinsic processability drawbacks that aqueous processable polymer such as poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) required cross-linkers to protect the thin film state from dissolution in aqueous environment, while glycolated polymers often counter marginal solubility problem in both organic and aqueous solvents. We show that the carboxylic acid-functionalized conjugated polyelectrolyte poly [3-(4-carboxypropyl) thiophene] (P3CPrT) can be processed from a water-soluble precursor, while requires no additives to yield solvent-resistant OECTs which exhibit electrochemical redox behavior in aqueous environment. In this study, we show P3CPrT OECTs exhibit unipolar p-type operation in accumulation mode which allows for much lower energy consumption compared with depletion mode, and the use of both interdigitated and planar OECTs for high transconductance behavior are demonstrated. Both physical and electrical properties are characterized to allow for a comparison with other high performing OMIECs. With the combination of advanced time-revolved structural and mass characterization techniques, namely Raman Spectroscopy and GiWAXs, and electrochemical quartz crystal microbalance with dissipation monitoring (EQCM-D), we provide insightful structure-property relationship for carboxylic-acid functionalized organic electrochemical transistor during electrochemical operation.

Time-revolved study on carboxylic-acid functionalized organic electrochemical transistor

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