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Solution-processed solid chitosan-based proton conductor film shows a large specific gate capacitance of ~7.47 μF/cm2 due to the interfacial electric-double-layer effect. Low-voltage (1.5 V) organic/inorganic hybrid transparent thin-film transistors with patterned indium-tin-oxide channels gated by chitosan films are self-assembled on glass substrates by only one metal shadow mask. The subthreshold gate voltage swing, current on/off ratio, and field-effect mobility are estimated to be 93 mV/dec, ~106, and 5.74 cm2·V-1·s-1, respectively. The reproducibility of pulse respond of such device is also demonstrated, which indicates the absence of electrochemical doping of the channel at the interface.