A 'Frugal' EGFET Sensor for Waterborne H2S.

Hydrogen sulphide (H2S) is a toxic gas soluble in water, H2Saq, as a weak acid. Since H2Saq usually originates from the decomposition of faecal matter, its presence also indicates sewage dumping and possible parallel waterborne pathogens associated with sewage. We here present a low footprint ('frugal') H2Saq sensor as an accessible resource for water quality monitoring. As a sensing mechanism, we find the chemical affinity of thiols to gold (Au) translates to H2Saq. When an Au electrode is used as a control gate (CG) or floating gate (FG) electrode in the electric double layer (EDL) pool of an extended gate field effect transistor (EGFET) sensor, EGFET transfer characteristics shift along the CG voltage axis in response to H2Saq. We rationalise this by the interface potential from the adsorption of polar H2S molecules to the electrode. The sign of the shift changes between Au CG and Au FG, and cancels when both electrodes are Au. The sensor is selective for H2Saq over the components of urine, nor does urine suppress the sensor's ability to detect H2Saq. Electrodes can be recovered for repeated use by washing in 1M HCl. Quantitatively, CG voltage shift is fitted by a Langmuir-Freundlich (LF) model, supporting dipole adsorption over an ionic (Nernstian) response mechanism. We find a limit-of-detection of 14.9 nM, 100 times below potability.

Bridged EGFET Design for the Rapid Screening of Sorbents as Sensitisers in Water-Pollution Sensors.

We further simplify the most 'user-friendly' potentiometric sensor for waterborne analytes, the 'extended-gate field effect transistor' (EGFET). This is accomplished using a 'bridge' design, that links two separate water pools, a 'control gate' (CG) pool and a 'floating gate' (FG) pool, by a bridge filled with agar-agar hydrogel. We show electric communication between electrodes in the pools across the gel bridge to the gate of an LND150 FET. When loading the gel bridge with a sorbent that is known to act as a sensitiser for Cu2+ water pollution, namely, the ion exchanging zeolite 'clinoptilolite', the bridged EGFET acts as a potentiometric sensor to waterborne Cu2+. We then introduce novel sensitisers into the gel bridge, the commercially available resins PurometTM MTS9140 and MTS9200, which are sorbents for the extraction of mercury (Hg2+) pollution from water. We find a response of the bridged EGFET to Hg2+ water pollution, setting a template for the rapid screening of ion exchange resins that are readily available for a wide range of harmful (or precious) metal ions. We fit the potentiometric sensor response vs. pollutant concentration characteristics to the Langmuir-Freundlich (LF) model which is discussed in context with other ion-sensor characteristics.

Exploring the ITO/PET Extended-Gate Field-Effect Transistor (EGFET) for pH Sensing.

In this project we investigated the extended-gate field-effect transistor (EGFET) structure used with ITO (Indium Tin Oxide)/PET (Polyethylene Terephthalate) sensitive films acting as the extended-gate part of an EGFET obtained from a combination of FETs from the CD4007 chip. We tested the device as a pH sensor by immersing the ITO/PET electrode in several chemical solutions of acidic and basic nature, including hydrogen peroxide, acetic acid, sulfuric acid, and ammonium hydroxide, at different concentrations. Using a Tektronix 4200A sourcemeter, we plotted the current-voltage (I-V) characteristics for the different chemical solutions, and we established a correlation to the pH changes. Results from the plotted I-V characteristics show a great dependance of the drain current (ID) on solution concentration. Furthermore, we measured the pH of each of the used solutions, and we established a relationship between the drain current and the pH value. Our results show a consistent decrease in the current with an increase in the pH value, although with different rates depending on the solution. The device showed high voltage sensitivity at 0.23 V per pH unit when tested in sulfuric acid.

The Characteristics Analysis of a Microfluid-Based EGFET Biosensor with On-Chip Sensing Film for Lactic Acid Detection.

In this research, a microfluid-based extended gate field-effect transistor (EGFET) biosensor with an on-chip sensing window (OCSW) was fabricated. The detection window was composed of six metal layers, and a ruthenium dioxide (RuO2) film was spattered on the surface and functionalized with lactase to detect lactic acid (LA). To detect LA in a more diversified way, a microfluidic system was integrated with the biosensor. Moreover, a special package was used to seal the sensing window and microfluidic tube and insulate it from other parts to prevent water molecule invasion and chip damage. The sensitivity analysis of the EGFET biosensor was studied by a semiconductor parameter analyzer (SPA). The static and dynamic measurements of the EGFET with sensing windows on a chip were analyzed. The sensing characteristics of the EGFET biosensor were verified by the experimental results. The proposed biosensor is suitable for wearable applications due to the advantages of its low weight, low voltage, and simple manufacturing process.

Sensitive pH measurement using EGFET pH-microsensor based on ZnO nanowire functionalized carbon-fibers.

Herein, we report the fabrication of zinc oxide nanowire (ZnO NW) coated carbon fiber (CF) ultra-microelectrodes (UME). ZnO NWs were grown on commercial multifilament CFs through hydrothermal process in a teflon-lined autoclave at 90 °C for 4 h. X-ray diffraction (XRD), Raman and scanning electron microscopy characterizations showed that crystalline and well oriented NW structures were successfully obtained. The fabrication of the pH sensitive UME was carried out by a novel approach which allowed controlling the protruding length of the modified CF surface. The UME was then integrated with a metal-oxide-semiconductor field effect transistor (MOSFET) for the construction of an EGFET pH-microsensor. The present pH microsensor is expected to be useful for localized pH measurement in small volumes such single cell analysis.

A Reliable BioFET Immunosensor for Detection of p53 Tumour Suppressor in Physiological-Like Environment.

The concentration of wild-type tumour suppressor p53wt in cells and blood has a clinical significance for early diagnosis of some types of cancer. We developed a disposable, label-free, field-effect transistor-based immunosensor (BioFET), able to detect p53wt in physiological buffer solutions, over a wide concentration range. Microfabricated, high-purity gold electrodes were used as single-use extended gates (EG), which avoid direct interaction between the transistor gate and the biological solution. Debye screening, which normally hampers target charge effect on the FET gate potential and, consequently, on the registered FET drain-source current, at physiological ionic strength, was overcome by incorporating a biomolecule-permeable polymer layer on the EG electrode surface. Determination of an unknown p53wt concentration was obtained by calibrating the variation of the FET threshold voltage versus the target molecule concentration in buffer solution, with a sensitivity of 1.5 ± 0.2 mV/decade. The BioFET specificity was assessed by control experiments with proteins that may unspecifically bind at the EG surface, while 100pM p53wt concentration was established as limit of detection. This work paves the way for fast and highly sensitive tools for p53wt detection in physiological fluids, which deserve much interest in early cancer diagnosis and prognosis.

Deep Submicron EGFET Based on Transistor Association Technique for Chemical Sensing.

Extended-gate field-effect transistor (EGFET) is an electronic interface originally developed as a substitute for an ion-sensitive field-effect transistor (ISFET). Although the literature shows that commercial off-the-shelf components are widely used for biosensor fabrication, studies on electronic interfaces are still scarce (e.g., noise processes, scaling). Therefore, the incorporation of a custom EGFET can lead to biosensors with optimized performance. In this paper, the design and characterization of a transistor association (TA)-based EGFET was investigated. Prototypes were manufactured using a 130 nm standard complementary metal-oxide semiconductor (CMOS) process and compared with devices presented in recent literature. A DC equivalence with the counterpart involving a single equivalent transistor was observed. Experimental results showed a power consumption of 24.99 mW at 1.2 V supply voltage with a minimum die area of 0.685 × 1.2 mm². The higher aspect ratio devices required a proportionally increased die area and power consumption. Conversely, the input-referred noise showed an opposite trend with a minimum of 176.4 nVrms over the 0.1 to 10 Hz frequency band for a higher aspect ratio. EGFET as a pH sensor presented further validation of the design with an average voltage sensitivity of 50.3 mV/pH, a maximum current sensitivity of 15.71 mA1/2/pH, a linearity higher than 99.9%, and the possibility of operating at a lower noise level with a compact design and a low complexity.

EGFET-Based Sensors for Bioanalytical Applications: A Review.

Since the 1970s, a great deal of attention has been paid to the development of semiconductor-based biosensors because of the numerous advantages they offer, including high sensitivity, faster response time, miniaturization, and low-cost manufacturing for quick biospecific analysis with reusable features. Commercial biosensors have become highly desirable in the fields of medicine, food, and environmental monitoring as well as military applications, whereas increasing concerns about food safety and health issues have resulted in the introduction of novel legislative standards for these sensors. Numerous devices have been developed for monitoring biological processes such as nucleic acid hybridization, protein⁻protein interaction, antigen⁻antibody bonds, and substrate⁻enzyme reactions, just to name a few. Since the 1980s, scientific interest moved to the development of semiconductor-based devices, which also include integrated front-end electronics, such as the extended-gate field-effect transistor (EGFET) biosensor, one of the first miniaturized chemical sensors. This work is intended to be a review of the state of the art focused on the development of biosensors and chemosensors based on extended-gate field-effect transistor within the field of bioanalytical applications, which will highlight the most recent research reported in the literature. Moreover, a comparison among the diverse EGFET devices will be presented, giving particular attention to the materials and technologies.

Frequency Response of Graphene Electrolyte-Gated Field-Effect Transistors.

This work develops the first frequency-dependent small-signal model for graphene electrolyte-gated field-effect transistors (EGFETs). Graphene EGFETs are microfabricated to measure intrinsic voltage gain, frequency response, and to develop a frequency-dependent small-signal model. The transfer function of the graphene EGFET small-signal model is found to contain a unique pole due to a resistive element, which stems from electrolyte gating. Intrinsic voltage gain, cutoff frequency, and transition frequency for the microfabricated graphene EGFETs are approximately 3.1 V/V, 1.9 kHz, and 6.9 kHz, respectively. This work marks a critical step in the development of high-speed chemical and biological sensors using graphene EGFETs.

Evaluation of sensitivity of Extended Gate Field Effect Transistor -biosensor based on V2O5/GOx for glucose detection.

The sensing modified electrode was prepared using glucose oxidase immobilized onto vanadium pentoxide xerogel with glass/FTO as support electrode to evaluate the possibility to construct a V2O5/GOx Extended Gate Field Effect Transistor biosensor. Previously, our studies exhibited a sensitivity of V2O5 of 58.1 mV/pH. The use of Nafion® onto V2O5/GOx caused a decrease of mass loss after several cycles compared to the modified electrode without Nafion® during the EQCM and cyclic voltammetrics studies. Electrical characterization of V2O5/GOx demonstrated a tendency to stability after 200 s as a function of applied current. In presence of glucose and in different pH, the current decreased when the glucose concentration increased due to the lower active sites of enzyme. After ten voltammetric cycles, the total charge tends to structural stability. In pH = 5.0, the modified electrode based on V2O5/GOx Extended Gate Field Effect Transistor presented more tendency to sensitivity in different concentration of glucose.

Brewer's Spent Grain-Cellulose-Coated Copper Electrode-Based Extended Gate Field-Effect Transistor for Nonenzymatic Glucose Detection toward Diagnosis of Diabetes Mellitus.

The demand for environmentally friendly, reliable, and cost-effective electrodes for glucose sensor technology has become a major research area in the paradigm shift toward green electronics. In this regard, cellulose has emerged as a promising flexible biopolymer solution with unique properties such as biocompatibility, biodegradability, nontoxicity, renewability, and sustainability. Because of their large surface area and porous structure, fibrous cellulose substrates quickly adsorb and disperse analytes at detection sites. This work focuses on utilizing glyoxal-treated cellulose (derived from brewer's spent grain (BSG)) for the fabrication of extended gate field-effect transistor (EGFET)-based glucose sensors. This investigation extends to the utilization of BSG-cellulose for glucose detection in biomimicking electrolytes (phosphate buffer saline) to facilitate glucose detection in human blood samples. The fabricated electrode demonstrates a linear range of glucose detection from 1 to 13.5 mM with a Langmuir adsorption coefficient (K) of 0.102. Also, its selectivity toward glucose over interfering molecules such as sucrose, fructose, ascorbic acid, and uric acid under physiological conditions has been demonstrated. This cellulose-based EGFET electrode exhibits a sensitivity of 6.5 µA mM-1 cm-2 with a limit of detection (LOD) of 0.135 mM. Computational studies by density functional theory calculations confirmed the higher binding affinity of glucose molecules with glyoxal-modified cellulose (-0.95 eV) than with pristine cellulose (-0.46 eV). Here, the novelty lies in the fabrication of electrodes with biodegradable catalysts and their integration into the EGFET configuration.

A simple and highly sensitive flexible sensor with extended-gate field-effect transistor for epinephrine detection utilizing InZnSnO sensing films.

This study introduces a straightforward method for depositing InZnSnO films onto flexible polyimide substrates at room temperature, enabling their application in electrochemical pH sensing and the detection of epinephrine. A comprehensive analysis of these sensing films, spanning structural, morphological, compositional, and profiling characteristics, was conducted using diverse techniques, including X-ray diffraction, atomic force microscopy, X-ray photoelectron spectroscopy, and secondary ion mass spectroscopy. The investigation into the influence of oxygen flow rates on the performance of InZnSnO sensitive films revealed a significant correlation between their structural properties and sensing capabilities. Notably, exposure to an oxygen flow rate of 30/2 (Ar/O2) the ratio of resulted in the InZnSnO sensitive film demonstrating outstanding pH sensitivity at 59.58 mV/pH within a broad pH range of 2-12, surpassing the performance observed with other oxygen flow rates. Moreover, under this specific condition, the film exhibited excellent stability, with a minimal drift rate of 0.14 mV/h at pH 7 and a low hysteresis voltage of 1.8 mV during a pH cycle of 7 â†’ 4→7 â†’ 10→7. Given the critical role of epinephrine in mammalian central nervous and hormone systems, monitoring its levels is essential for assessing human health. To facilitate the detection of epinephrine, we utilized the carboxyl group of 4-formylphenylboronic acid to enable a reaction with the amino group of the 3-aminopropyltriethoxysilane-coated InZnSnO film. Through optimization, the resulting InZnSnO-based flexible sensor displayed a broad and well-defined linear relationship within the concentration range of 10-7 to 0.1 µM. In practical applications, this sensor proved effective in analyzing epinephrine in human serum, showcasing notable selectivity, stability, and reproducibility. The promising outcomes of this study underscore the potential for future applications, leveraging the advantages of electrochemical sensors, including affordability, rapid response, and user-friendly operation.

Pyrene Derivative Incorporated Ni MOF as an Enzyme Mimic for Noninvasive Salivary Glucose Detection Toward Diagnosis of Diabetes Mellitus.

Herein, we demonstrate the detection of glucose in a noninvasive and nonenzymatic manner by utilizing an extended gate field-effect transistor (EGFET) based on the organic molecule pyrene phosphonic acid (PyP4OH8) incorporated nickel metal-organic framework (NiOM-MOF). The prepared electrode responds selectively to glucose instead of sucrose, fructose, maltose, ascorbic acid, and uric acid in a 1× phosphate buffer saline solution. Also, utilizing the scanning Kelvin probe system, the sensing electrode's work function (Φ) is measured to validate the glucose-sensing mechanism. The sensitivity, detection range, response time, limit of detection, and limit of quantification of the electrode are determined to be 24.5 µA mM-1 cm-2, 20 µM to 10 mM, less than 5 s, 2.73 µM, and 8.27 µM, respectively. Most interestingly, the developed electrode follows the Michaelis-Menten kinetics, and the calculated rate constant (km) 0.07 mM indicates a higher affinity of NiOM-MOF toward glucose. The real-time analysis has revealed that the prepared electrode is sensitive to detect glucose in real human saliva, and it can be an alternative device for the noninvasive detection of glucose. Overall, the outcomes of the EGFET studies demonstrate that the prepared electrodes are well-suited for expeditious detection of glucose levels in saliva.

The Integration of Field Effect Transistors to Microfluidic Devices.

Devices that integrate field effect transistors into microfluidic channels are becoming increasingly promising in the medical, environmental, and food realms, among other applications. The uniqueness of this type of sensor lies in its ability to reduce the background signals existing in the measurements, which interfere in obtaining good limits of detection for the target analyte. This and other advantages intensify the development of selective new sensors and biosensors with coupling configuration. This review work focused on the main advances in the fabrication and application of field effect transistors integrated into microfluidic devices as a way of identifying the potentialities that exist in these systems when used in chemical and biochemical analyses. The emergence of research on integrated sensors is not a recent study, although more recently the progress of these devices is more accentuated. Among the studies that used integrated sensors with electrical and microfluidic parts, those that investigated protein binding interactions seem to be the ones that expanded the most due, among other things, to the possibility of obtaining several physicochemical parameters involved in protein-protein interactions. Studies in this area have a great possibility of advancing innovations in sensors with electrical and microfluidic interfaces in new designs and applications.

Effect of Microwave Annealing on the Sensing Characteristics of HfO2 Thin Film for High Sensitive pH-EGFET Sensor.

Recently, certain challenges have persisted in PH sensor applications, especially when employing hafnium oxide (HfO2) thin films as sensing layers, where issues related to sensitivity, hysteresis, and long-term stability hamper performance. Microwave annealing (MWA) technology, as a promising solution for addressing these challenges, has gained significant attraction due to its unique advantages. In this article, the effects of microwave annealing (MWA) treatment on the sensing behaviors of Extended-Gate Field-Effect Transistors (EGFETs) utilizing HfO2 as a sensing film have been investigated for the first time. Various power levels of MWA treatment (1750 W/2100 W/2450 W) were selected to explore the optimal processing conditions. A thorough physical analysis was conducted to characterize the surface of the MWA-treated HfO2 sensing thin film using techniques such as X-ray photoelectron spectroscopy (XPS) and atomic force microscopy (AFM). Our findings reveal that MWA treatment effectively increased the surface sites (Ns) in the HfO2 sensing thin film, consequently leading to an increase in the pH sensitivity of EGFETs to 59.6 mV/pH, as well as a reduction in hysteresis and an enhancement in long-term stability. These results suggest that MWA offers a straightforward, energy-efficient method to enhance overall HfO2 sensing film performance in EGFETs, offering insights for HfO2 applications and broader microelectronics challenges.

Sensitivity of Al-Doped Zinc-Oxide Extended Gate Field Effect Transistors to Low-Dose X-ray Radiation.

Herein, we investigated the applicability of thick film and bulk disk forms of aluminum-doped zinc oxide (AZO) for low-dose X-ray radiation dosimetry using the extended gate field effect transistor (EGFET) configuration. The samples were fabricated using the chemical bath deposition (CBD) technique. A thick film of AZO was deposited on a glass substrate, while the bulk disk form was prepared by pressing the collected powders. The prepared samples were characterized via X-ray diffraction (XRD) and field emission scanning electron microscope (FESEM) to determine the crystallinity and surface morphology. The analyses show that the samples are crystalline and comprise nanosheets of varying sizes. The EGFET devices were exposed to different X-ray radiation doses, then characterized by measuring the I-V characteristics pre- and post-irradiation. The measurements revealed an increase in the values of drain-source currents with radiation doses. To study the detection efficiency of the device, various bias voltages were also tested for the linear and saturation regimes. Performance parameters of the devices, such as sensitivity to X-radiation exposure and different gate bias voltage, were found to depend highly on the device geometry. The bulk disk type appears to be more radiation-sensitive than the AZO thick film. Furthermore, boosting the bias voltage increased the sensitivity of both devices.

Highly Sensitive and Selective Sol-Gel Spin-Coated Composite TiO2-PANI Thin Films for EGFET-pH Sensor.

A highly selective and sensitive EGFET-pH sensor based on composite TiO2-PANI had been developed in this work. A sol-gel titanium dioxide (TiO2) and the composite of TiO2 with semiconducting polyaniline (PANI) were deposited using a simple spin-coating method on an indium tin oxide (ITO) substrate. The films have been explored as a sensing electrode (SE) of extended gate field-effect transistor (EGFET) for pH applications in the range of pH 2 to 12. The pH sensitivities between TiO2, TiO2-PANI bilayer composite, and TiO2-PANI composite thin films were discussed. Among these, the TiO2-PANI composite thin film showed a super-Nernstian behavior with high sensitivity of 66.1 mV/pH and linearity of 0.9931; good repeatability with a standard deviation of 0.49%; a low hysteresis value of 3 mV; and drift rates of 4.96, 5.54, and 3.32 mV/h in pH 4, 7, and 10, respectively, for 6 h. Upon applying the TiO2-PANI composite as the SE for nitrate measurement, low sensitivity of 12.9 mV/dec was obtained, indicating that this film is a highly selective sensing electrode as a pH sensor. The surface morphology and crystallinity of the thin films were also discussed.

Molecularly imprinted polymer-based extended-gate field-effect transistor (EG-FET) chemosensor for selective determination of matrix metalloproteinase-1 (MMP-1) protein.

A conducting molecularly imprinted polymer (MIP) film was integrated with an extended-gate field-effect transistor (EG-FET) transducer to determine epitopes of matrix metalloproteinase-1 (MMP-1) protein biomarker of idiopathic pulmonary fibrosis (IPF) selectively. Most suitable epitopes for imprinting were selected with Basic Local Alignment Search Tool software. From a pool of MMP-1 epitopes, the two, i.e., MIAHDFPGIGHK and HGYPKDIYSS, the relatively short ones, most promising for MMP-1 determination, were selected, mainly considering their advantageous outermost location in the protein molecule and stability against aggregation. MIPs templated with selected epitopes of the MMP-1 protein were successfully prepared by potentiodynamic electropolymerization and simultaneously deposited as thin films on electrodes. The chemosensors, constructed of MIP films integrated with EG-FET, proved useful in determining these epitopes even in a medium as complex as a control serum. The limit of detection for the MIAHDFPGIGHK and HGYPKDIYSS epitope was ∼60 and 20 nM, respectively. Moreover, the chemosensors selectively recognized whole MMP-1 protein in the 50-500 nM concentration range in buffered control serum samples.

Rapid and label-free detection of the troponin in human serum by a TiN-based extended-gate field-effect transistor biosensor.

In this article, the TiN sensitive film as a sensing membrane was deposited onto n+-type Si substrate by a DC sputtering technique for extended-gate field-effect transistor (EGFET) pH sensors and detection of cardiac troponin-I (cTn-I) in the patient sera for the first time. The crystal structure, Raman spectrum, element profile, surface roughness, and surface morphology of the TiN sensitive film were characterized by X-ray diffraction, Raman spectroscopy, secondary ion mass spectroscopy, atomic force microscopy, and scanning electron microscopy, respectively. The sensing performance of the TiN sensitive film is correlated with its relative structural feature. A high sensitivity of 57.49 mV/pH, a small hysteresis voltage of ∼1 mV, and a low drift rate of 0.31 mV/h were obtained in the TiN sensitive film. In addition, the pH sensitivity of this TiN EGFET sensor was preserved approximately 57 mV/pH after operation time of 180 days. Subsequently, the cTn-I antibodies with carboxyl groups activated by 1-ethyl-3-(3-dimethylaminopropyl)-carbodiimide (EDC) along with N-hydroxysuccinimide (NHS) were immobilized on the TiN sensitive film functionalizing with 3-aminopropyl triethoxysilane (APTES). After obtaining the successful immobilization of cTn-I antibodies on the TiN EGFET biosensor, the cTn-I antigen specifically binds with its relative antibody. The cTn-I EGFET biosensor showed a high sensitivity of 21.88 mV/pCcTn-I in a wide dynamic range of 0.01-100 ng/mL. Furthermore, the concentrations of cTn-I in patient sera measured by our TiN EGFET biosensors are comparable to those determined by commercial enzyme-linked immuno-sorbent assay kits.

Field-Effect Transistor with a Plasmonic Fiber Optic Gate Electrode as a Multivariable Biosensor Device.

A novel multivariable system, combining a transistor with fiber optic-based surface plasmon resonance spectroscopy with the gate electrode simultaneously acting as the fiber optic sensor surface, is reported. The dual-mode sensor allows for discrimination of mass and charge contributions for binding assays on the same sensor surface. Furthermore, we optimize the sensor geometry by investigating the influence of the fiber area to transistor channel area ratio and distance. We show that larger fiber optic tip diameters are favorable for electronic and optical signals and demonstrate the reversibility of plasmon resonance wavelength shifts after electric field application. As a proof of principle, a layer-by-layer assembly of polyelectrolytes is performed to benchmark the system against multivariable sensing platforms with planar surface plasmon resonance configurations. Furthermore, the biosensing performance is assessed using a thrombin binding assay with surface-immobilized aptamers as receptors, allowing for the detection of medically relevant thrombin concentrations.