Synergistic Effect of Oxoammonium Salt and Its Counterions for Fabricating Organic Electrochemical Transistors with Low Power Consumption

The state-of-the-art poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS)-based organic electrochemical transistors (OECTs) are gaining importance for a variety of biological applications due to their mixed electronic and ionic conductivities featuring ion-to-electron conversion. A low operation voltage without sacrificing device performance is desired to realize long-term monitoring of biological activities. In the present work, oxoammonium salts with two different counterions (TEMPO+X–, where TEMPO = 2,2,6,6-tetramethylpiperidine-1-oxoammonium; X = Br– and TFSI–) are employed as secondary dopants to modulate the device performance. Both oxoammonium salts feature a distinct dopant concentration-dependent doping effect, allowing precise control in improving the performance of OECTs. A zero-gate bias, corresponding to the maximum transconductance, and a low threshold voltage are realized by optimizing the dopant concentrations. In addition, TEMPO+TFSI– dopant exerts great capability in modulating the work function and in morphology reconstruction of PEDOT:PSS, ensuring a well-matched work function at the gold electrode–channel material interface and condensed microstructure stacking with an edge-on orientation in the doped PEDOT:PSS films. The synergistic effect of TEMPO and the TFSI– counterion endows the device with superior performance to its counterparts due to the resultant higher μC* figure, benefiting from the efficient injection/extraction of holes at the interface and enhanced intra- and inter-chain carrier transport. The excellent device performance makes the OECT a promising neuromorphic device to mimic basic brain functions.