Field-effect transistor-based biosensors (bio-FETs) are promising candidates for the rapid high-sensitivity and high-selectivity sensing of various analytes in healthcare, clinical diagnostics, and the food industry. However, bio-FETs still have several unresolved problems that hinder their technological transfer, such as electrical stability. Therefore, it is important to develop reliable, efficient devices and establish facile electrochemical characterization methods. In this work, we have fabricated a flexible biosensor based on an Al:ZnO thin-film transistor (TFT) gated through an aqueous electrolyte on a polyimide substrate. In addition, we demonstrated techniques for establishing the operating range of such devices. The Al:ZnO-based devices with a channel length/width ratio of 12.35 and a channel thickness of 50 nm were produced at room temperature via magnetron sputtering. These Al:ZnO-based devices exhibited high field-effect mobility (μ = 6.85 cm2/Vs) and threshold voltage (Vth = 654 mV), thus showing promise for application on temperature-sensitive substrates. X-ray photoelectron spectroscopy was used to verify the chemical composition of the deposited films, while the morphological aspects of the films were assessed using scanning electron and atomic force microscopies. The gate–channel electric capacitance of 40 nF/cm2 was determined using electrochemical impedance spectroscopy, while the electrochemical window of the gate–channel system was determined as 1.8 V (from −0.6 V to +1.2 V) using cyclic voltammetry. A deionized water solution of 10 mer (CCC AAG GTC C) DNA aptamer (molar weight −2972.9 g/mol) in a concentration ranging from 1–1000 pM/μL was used as an analyte. An increase in aptamer concentration caused a proportional decrease in the TFT channel conductivity. The techniques demonstrated in this work can be applied to optimize the operating parameters of various semiconductor materials in order to create a universal detection platform for biosensing applications, such as multi-element FET sensor arrays based on various composition nanostructured films, which use advanced neural network signal processing.
This research presents a comparative analysis of water-gated thin film transistors based on a copper oxide (CuO) semiconductor in the form of a smooth film and a nanostructured surface. A smooth CuO film was deposited through reactive magnetron sputtering followed by annealing in atmosphere at a temperature of 280 ∘C. Copper oxide nanostructures were obtained by hydrothermal synthesis on a preliminary magnetron sputtered 2 nm thick CuO precursor followed by annealing at 280 ∘C. An X-ray diffraction (XRD) analysis of the samples revealed the presence of a tenorite (CuO) phase with a predominant orientation of (002). Scanning electron microscopy (SEM) and atomic force microscopy (AFM) studies of the samples revealed a highly developed surface with crystallites having a monoclinic syngony and dimensions of 15–20 nm in thickness, 150 nm in length, and 100 nm in height relative to a 2.5 nm height for the CuO crystallites of the smooth film. Electric measurements of the studied devices revealed typical current–voltage characteristics of semiconductors with predominant hole conductivity. The maximum ON/OFF ratio at a rain-source voltage of 0.4 volts and −1.2 volts on the gate for a smooth film was 102, and for a nanostructured transistor, it was 103. However, a much stronger saturation of the channel was observed for the nanostructured channel than for the smooth film. A test solution containing glyphosate dissolved in deionized water in three different concentrations of 5, 10, and 15 μmol/L was used during the experiments. The principle of operation was based on the preliminary saturation of the solution with Cu ions, followed by the formation of a metal–organic complex alongside glyphate. The glyphosate contents in the analyte led to a decrease in the conductivity of the transistor on the axis of the smooth film. In turn, the opposite effect was observed on the nanostructured surface, i.e., an increase in conductivity was noted upon the introduction of an analyte. Despite this, the overall sensitivity of the nanostructured device was twice as high as that of the device with a thin film channel. The relative changes in the field-effect transistor (FET) conductivity at maximum glyphosate concentrations of 15 μmol/L reached 19.42% for the nanostructured CuO film and 3.3% for the smooth film.
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