Liquid-gated Field-effect Transistor Research Articles

Comparative Study of Field-Effect Transistors Based on Graphene Oxide and CVD Graphene in Highly Sensitive NT-proBNP Aptasensors.

Graphene-based materials are actively being investigated as sensing elements for the detection of different analytes. Both graphene grown by chemical vapor deposition (CVD) and graphene oxide (GO) produced by the modified Hummers' method are actively used in the development of biosensors. The production costs of CVD graphene- and GO-based sensors are similar; however, the question remains regarding the most efficient graphene-based material for the construction of point-of-care diagnostic devices. To this end, in this work, we compare CVD graphene aptasensors with the aptasensors based on reduced GO (rGO) for their capabilities in the detection of NT-proBNP, which serves as the gold standard biomarker for heart failure. Both types of aptasensors were developed using commercial gold interdigitated electrodes (IDEs) with either CVD graphene or GO formed on top as a channel of liquid-gated field-effect transistor (FET), yielding GFET and rGO-FET sensors, respectively. The functional properties of the two types of aptasensors were compared. Both demonstrate good dynamic range from 10 fg/mL to 100 pg/mL. The limit of detection for NT-proBNP in artificial saliva was 100 fg/mL and 1 pg/mL for rGO-FET- and GFET-based aptasensors, respectively. While CVD GFET demonstrates less variations in parameters, higher sensitivity was demonstrated by the rGO-FET due to its higher roughness and larger bandgap. The demonstrated low cost and scalability of technology for both types of graphene-based aptasensors may be applicable for the development of different graphene-based biosensors for rapid, stable, on-site, and highly sensitive detection of diverse biochemical markers.

Femtomolar detection of the heart failure biomarker NT-proBNP in artificial saliva using an immersible liquid-gated aptasensor with reduced graphene oxide

Measuring NT-proBNP biomarker is recommended for preliminary diagnostics of the heart failure. Recent studies suggest a possibility of early screening of biomarkers in saliva for non-invasive identification of cardiac diseases at the point-of-care. However, NT-proBNP concentrations in saliva can be thousand time lower than in blood plasma, going down to pg/mL level. To reach this level, we developed a label-free aptasensor based on a liquid-gated field effect transistor using a film of reduced graphene oxide monolayer (rGO-FET) with immobilized NT-proBNP specific aptamer. We found that, depending on ionic strength of tested solutions, there were different levels of correlation in responses of electrical parameters of the rGO-FET aptasensor, namely, the Dirac point shift and transconductance change. The correlation in response to NT-proBNP was high for 1.6 mM phosphate-buffered saline (PBS) and zero for 16 mM PBS in a wide range of analyte concentrations, varied from 1 fg/mL to 10 ng/mL. The effects of transconductance and Dirac point shift in PBS solutions of different concentrations are discussed. The biosensor exhibited a high sensitivity for both transconductance (2 µS/decade) and Dirac point shift (2.3 mV/decade) in diluted PBS with the linear range from 10 fg/mL to 1 pg/mL. The aptasensor performance has been also demonstrated in undiluted artificial saliva with the achieved limit of detection down to 41 fg/mL (∼4.6 fM).

Formation of Highly Conductive Interfaces in Crystalline Ionic Liquid-Gated Unipolar MoTe2/h-BN Field-Effect Transistor.

2H MoTe2 (molybdenum ditelluride) has generated significant interest because of its superconducting, nonvolatile memory, and semiconducting of new materials, and it has a large range of electrical properties. The combination of transition metal dichalcogenides (TMDCs) and two dimensional (2D) materials like hexagonal boron nitride (h-BN) in lateral heterostructures offers a unique platform for designing and engineering novel electronic devices. We report the fabrication of highly conductive interfaces in crystalline ionic liquid-gated (ILG) field-effect transistors (FETs) consisting of a few layers of MoTe2/h-BN heterojunctions. In our initial exploration of tellurium-based semiconducting TMDs, we directed our attention to MoTe2 crystals with thicknesses exceeding 12 nm. Our primary focus centered on investigating the transport characteristics and quantitatively assessing the surface interface heterostructure. Our transconductance (gm) measurements indicate that the very efficient carrier modulation with an ILG FET is two times larger than standard back gating, and it demonstrates unipolarity of the device. The ILG FET exhibited highly unipolar p-type behavior with a high on/off ratio, and it significantly increased the mobility in MoTe2/h-BN heterochannels, achieving improvement as one of the highest recorded mobility increments. Specifically, we observed hole and electron mobility values ranging from 345 cm2 V-1 s-1 to 285 cm2 V-1 s-1 at 80 K. We predict that our ability to observe the intrinsic, heterointerface conduction in the channels was due to a drastic reduction of the Schottky barriers, and electrostatic gating is suggested as a method for controlling the phase transitions in the few layers of TMDC FETs. Moreover, the simultaneous structural phase transitions throughout the sample, achieved through electrostatic doping control, presents new opportunities for developing phase change devices using atomically thin membranes.

High-Pressure Synthesis of Single-Crystalline SnS Nanoribbons.

Two-dimensional tin monosulfide (SnS) is attractive for the development of electronic and optoelectronic devices with anisotropic characteristics. However, its shape-controlled synthesis with an atomic thickness and high quality remains challenging. Here, we show that highly crystalline SnS nanoribbons can be produced via high-pressure (0.5 GPa) and thermal treatment (400 °C). These SnS nanoribbons have a length of several tens of micrometers and a thickness down to 5.8 nm, giving an average aspect ratio of ∼30.6. The crystal orientation along the zigzag direction and the in-plane structural anisotropy of the SnS nanoribbons are identified by transmission electron microscopy and polarized Raman spectroscopy, respectively. An ionic liquid-gated field-effect transistor fabricated using the SnS nanoribbon exhibits an on/off current ratio of >103 and a field-effect mobility of ∼0.7 cm2 V-1 s-1. This work provides a unique way to achieve one-dimensional growth of SnS.

The Significance of Nonlinear Screening and the pH Interference Mechanism in Field-Effect Transistor Molecular Sensors.

Electrolyte screening is well known for its detrimental impact on the sensitivity of liquid-gated field-effect transistor (FET) molecular sensors and is mostly described by the linearized Debye-Hückel model. However, charged and pH-sensitive FET sensing surfaces can limit the FET molecular sensitivity beyond the Debye-Hückel screening formalism. Pre-existing surface charges can lead to the breakdown of Debye-Hückel screening and induce enhanced nonlinear Poisson-Boltzmann screening. Moreover, the charging of the pH-sensitive surface groups interferes with biomolecule sensing resulting in a pH interference mechanism. With analytical equations and TCAD simulations, we highlight that the Debye-Hückel approximation can underestimate screening and overestimate FET molecular sensitivity by more than an order of magnitude. Screening strengthens significantly beyond Debye-Hückel in the proximity of even moderately charged surfaces and biomolecule charge densities (≥1 × 1012 q/cm2). We experimentally show the strong impact of both nonlinear screening and the pH interference effect on charge-based biomolecular sensing using a model system based on the covalent binding of single-stranded DNA on silicon FET sensors. The DNA signal increases from 24 mV at pH 7 to 96 mV at pH 3 in 1.5 mM PBS for a DNA density of 7 × 1012 DNA/cm2. Our model quantitatively explains the signal's pH dependence with roughly equal nonlinear screening and pH interference contributions. This work shows the importance of reducing the net charge and the pH sensitivity of the sensing surface to improve molecular sensing. Therefore, tailoring the gate dielectric and functional layer of FET sensors is a promising route to strong silicon FET molecular sensitivity boosts.

Electron and hole mobilities in ambipolar MoS2 electric-double-layer transistor

We report transport measurements of ionic liquid-gated field-effect transistors with multilayer MoS2 channels. Ambipolar characteristics with high ON/OFF ratios (>105) are observed. The current–voltage characteristics agree well with those calculated using a simple model assuming a high recombination probability and negligible contact resistance, except when holes are doped in the vicinity of the source contact. Electron and hole mobilities are estimated using the current–voltage characteristics in both the unipolar and ambipolar modes, wherein a p–n junction is formed in the latter. The electron mobility depends significantly on the carrier distribution in a channel that is controlled by the gate voltage. This result is attributed to the significant field dependence of the electron mobility.

(Nano 2nd Place Best Poster Winner) Fabrication of Nanocarbon-Based Field-Effect Transistor Biosensors for Electronic Detection of DNA Sequences

We report on the design and assembly of liquid-gated field-effect transistor devices based on graphene nanoribbons, G-FETs, their functionalization with anchor groups, as well as their response to single-stranded DNA probe tethering and complementary DNA target hybridization in saline buffer solution. The probe DNA was immobilized onto the graphene surface by covalent functionalization with aryldiazonium chemistry. We characterized the electrical response of the devices before and after functionalization. DNA probe tethering and target hybridization were monitored by shifts of the charge neutrality point. Additionally, the electrical response to probe immobilization and probe-target hybridization was recorded in real-time.

Immobilization of glucose oxidase on ZnO nanorods decorated electrolyte-gated field effect transistor for glucose detection

In this paper, we report on growth of ZnO nanorods on the surface of gold interdigital electrodes and its implementation as a conductive n-type channel for the fabrication of a liquid-gated field effect transistor. Glucose oxidase was immobilized on the surface of the ZnO nanorods and the fabricated device was used as a four-electrode glucose biosensor. The resistance of the conductive channel was affected by addition of glucose. The applied bias voltage to the gate in the fabricated device affects the channel resistance in the same manner as the increase of enzymatic products during the glucose oxidation. Large effective area, good conductivity, and biocompatibility properties of ZnO nanorods are the key features in this highly sensitive and stable biosensor. Our measurements showed that the threshold voltage of transistor was about 0.75 V. The current increased in the presence of the glucose and exhibited a dynamic linear range with the logarithm of glucose concentration in the range between 0.01 and 5 mM. The detection limit was about 3.8 μM.

Large scale commercial fabrication of high quality graphene-based assays for biomolecule detection

Large numbers of high quality graphene transistors with mobility approximately 5000cm2/V*s were fabricated by chemical vapor deposition and packaged into ceramic carriers with an open cavity design. The ceramic carrier is compatible with standard electronics assembly, enabling the readout of graphene properties on the benchtop without large, expensive probing systems. After chemical functionalization, these sensors demonstrate sensitivity in the pM range and selectivity to many classes of biomolecules as a three terminal liquid-gated field effect transistor. High precision measurements of protein kinetics captured using this technology, commercially known as AGILE R100, are comparable and can exceed the capabilities of state-of-the-art biomolecule characterization tools.

Ionic screening effect on low-frequency drain current fluctuations in liquid-gated nanowire FETs

The ionic screening effect plays an important role in determining the fundamental surface properties within liquid–semiconductor interfaces. In this study, we investigated the characteristics of low-frequency drain current noise in liquid-gated nanowire (NW) field effect transistors (FETs) to obtain physical insight into the effect of ionic screening on low-frequency current fluctuation. When the NW FET was operated close to the gate voltage corresponding to the maximum transconductance, the magnitude of the low-frequency noise for the NW exposed to a low-ionic-strength buffer (0.001 M) was approximately 70% greater than that when exposed to a high-ionic-strength buffer (0.1 M). We propose a noise model, considering the charge coupling efficiency associated with the screening competition between the electrolyte buffer and the NW, to describe the ionic screening effect on the low-frequency drain current noise in liquid-gated NW FET systems. This report not only provides a physical understanding of the ionic screening effect behind the low-frequency current noise in liquid-gated FETs but also offers useful information for developing the technology of NW FETs with liquid-gated architectures for application in bioelectronics, nanosensors, and hybrid nanoelectronics.

Label-free electronic detection of interleukin-6 using horizontally aligned carbon nanotubes

A facile, sensitive, and label-free assay for detection of interleukin-6 (IL-6) using liquid-gated field-effect transistor (FET) sensors based on horizontally aligned single-walled carbon nanotubes (SWCNT) is proposed. This approach relies on the drain current (Id) responses of the transistor upon interactions of IL-6 with its corresponding antibody (IL-6R) immobilized on SWCNT. The proposed immunosensor exhibits superior sensitivity (limit-of-detection=1.37pg/mL) in virtue of the reduced tube-to-tube contact resistance, good selectivity (no responses to bovine serum albumin and cysteine were observed and detection of target molecules in serum was achieved) as a result of the highly specific interaction between IL-6 and IL-6R, and excellent stability (no significant degradation in the electronic performance after storage under ambient conditions for up to 3months) in virtue of the strong adhesion of CNT to the quartz substrate and good horizontal alignment of these tubes. Therefore, the proposed immunosensor is a promising platform for early diagnosis of various diseases (including some cancers) that can be indicated by the circulating level of IL-6.

Electrostatically induced superconductivity at the surface of WS₂.

We investigate transport through ionic liquid gated field effect transistors (FETs) based on exfoliated crystals of semiconducting WS2. Upon electron accumulation, at surface densities close to, or just larger than, 10(14) cm(-2), transport exhibits metallic behavior with the surface resistivity decreasing pronouncedly upon cooling. A detailed characterization as a function of temperature and magnetic field clearly shows the occurrence of a gate-induced superconducting transition below a critical temperature Tc ≈ 4 K, a finding that represents the first demonstration of superconductivity in tungsten-based semiconducting transition metal dichalcogenides. We investigate the nature of superconductivity and find significant inhomogeneity, originating from the local detaching of the frozen ionic liquid from the WS2 surface. Despite the inhomogeneity, we find that in all cases where a fully developed zero resistance state is observed, different properties of the devices exhibit a behavior characteristic of a Berezinskii-Kosterlitz-Thouless transition, as it could be expected in view of the two-dimensional nature of the electrostatically accumulated electron system.

Ionic Liquid versus SiO2 Gated a-IGZO Thin Film Transistors: A Direct Comparison

Ionic liquid gated field effect transistors have been extensively studied due to their low operation voltage, ease of processing and the realization of high electric fields at low bias voltages. Here, we report ionic liquid (IL) gated thin film transistors (TFTs) based on amorphous Indium Gallium Zinc Oxide (a-IGZO) active layers and directly compare the characteristics with a standard SiO2 gated device. The transport measurements of the top IL gated device revealed the n-channel property of the IGZO thin film with a current ON/OFF ratio ∼105, a promising field effect mobility of 14.20 cm2V−1s−1, and a threshold voltage of 0.5 V. Comparable measurements on the bottom SiO2 gate insulator revealed a current ON/OFF ratio >108, a field effect mobility of 13.89 cm2V−1s−1 and a threshold voltage of 2.5 V. Furthermore, temperature-dependent measurements revealed that the ionic liquid electric double layer can be “frozen-in” by cooling below the glass transition temperature with an applied electrical bias. Positive and negative freezing bias locks-in the IGZO TFT “ON” and “OFF” state, respectively, which could lead to new switching and possibly non-volatile memory applications.

Scanning photocurrent microscopy reveals electron-hole asymmetry in ionic liquid-gated WS2 transistors

We perform scanning photocurrent microscopy on WS2 ionic liquid-gated field effect transistors exhibiting high-quality ambipolar transport. By properly biasing the gate electrode, we can invert the sign of the photocurrent showing that the minority photocarriers are either electrons or holes. Both in the electron- and hole-doping regimes the photocurrent decays exponentially as a function of the distance between the illumination spot and the nearest contact, in agreement with a two-terminal Schottky-barrier device model. This allows us to compare the value and the doping dependence of the diffusion length of the minority electrons and holes on a same sample. Interestingly, the diffusion length of the minority carriers is several times larger in the hole accumulation regime than in the electron accumulation regime, pointing out an electron-hole asymmetry in WS2.

Analytical prediction of liquid-gated graphene nanoscroll biosensor performance

The latest discovery of the graphene nanoscroll has provided enormous new stimuli to carbon nanoresearch. Due to its one-dimensional structure and tunable core size, the graphene nanoscroll is suitable for nanoscale applications such as in nanotransistors, and biosensor devices. DNA sensing is critical in the identification of the genetic risk factors associated with complex human diseases, and continues to have an emerging role in therapeutics and personalized medicine. This paper presents the analytical model of liquid-gated field effect transistors (LGFETs) for zig-zag graphene nanoscrolls (ZGNSs) inspired by carbon nanotube behavior when exposed to DNA molecules. First of all, in order to gain physical insight into GNS-based devices, the conductance of GNSs is analytically modelled. Based on the sensing mechanism of the DNA sensor, GNS controlling elements (ηGNS and eGNS) are proposed and the behavior of LGFETs-based GNS nanomaterial in the presence of DNA molecules is predicted to get a greater insight into the rapid development of DNA sensors and their application. Because of the channel-doping effect due to the adsorption of the DNA molecules, the conductance of the channel is altered. On the other hand, the applied voltage effect in the form of tilted electron energy levels is utilized in the form of normalized Fermi energy variation which is used in the sensor modelling. This study emphasizes the promising nature of carbon nanoscrolls for a number of electronic device applications.

High-Yield Fabrication of Graphene Chemiresistors With Dielectrophoresis

We demonstrate a simple, low-cost, but effective approach to deposit graphene on silicon wafers with dielectrophoresis. With a comb-shaped electrode design, graphene sheets can be actively captured between electrodes. Dielectrophoresis proves effective in depositing a large-scale array of graphene on desired locations. The deposition of semiconducting single-walled carbon nanotubes (s-SWNTs) with the same approach is also studied to compare the two forms of carbon-based nanomaterials. The graphene deposition has a lower success rate (approximately 62%) than s-SWNTs (100%) to cover the comb fingers due to the 2-D sheet structure and larger dimensions of the material. The assembled graphene sheets can successfully bridge over the electrode gap to create functional, ready-to-use electronic devices. The dielectrophoretically deposited graphene is used as the semiconducting material in a liquid-gated field-effect transistor, and it demonstrates p-type characteristics with holes as the majority charge carriers. When used in two-terminal chemiresistors, the deposited graphene demonstrates high sensitivity toward pH values in liquid. The resistance of graphene is inversely proportional to the pH value of the solution in the range of 5-9 with the pH sensitivity of 17.5 Ω/decade. The high-precision, high-yield deposition provides a practical approach for the fabrication of future graphene electronic devices and sensors.

Enzyme-Free Sugar Sensing in Microfluidic Channels with an Affinity-Based Single-Wall Carbon Nanotube Sensor

We present a novel nonenzymatic carbon nanotube sensor integrated in a microfluidic channel for the detection of sugars. The sensor is assembled as a liquid-gated field-effect transistor, with the transistor channel composed of 1 to 10 nanotubes, which are controllably functionalized with boronic acid receptors. The devices show sensitivity to glucose in a concentration range of 5 to 30 mM. Furthermore, by controlling the type of nanotube-receptor coupling (as covalent or noncovalent) and by deploying a sensitive impedance-based detection technique, we corroborate in detail the transduction mechanism of our affinity-based sensor. In the case of covalent coupling, charge carrier scattering along the nanotubes is the dominant mechanism. While in the noncovalent case, surface charge effects dominate. The identification of the mechanism along with the tunability of the chemical coupling and the cost-effective integration in microchannels constitute a solid basis for the entry of nanotube-based sensors in lab-on-a-chip applications.

Nanotubes-/nanowires-based, microfluidic-integrated transistors for detecting biomolecules

Nanotubes and nanowires have sparked considerable interest in biosensing applications due to their exceptional charge transport properties and size compatibility with biomolecules. Among the various biosensing methodologies incorporating these nanostructured materials in their sensing platforms, liquid-gated field-effect transistors (LGFETs)-based device configurations outperform the conventional electrochemical measurements by their ability in providing label free, direct electronic read-out, and real-time detection. Together with integration of a microfluidic channel into the device architecture, nanotube- or nanowires-based LGFET biosensor have demonstrated promising potential toward the realization of truly field-deployable self-contained lab-on-chip devices, which aim to complement the existing lab-based methodologies. This review addresses the recent advances in microfluidic-integrated carbon nanotubes and inorganic nanowires-based LGFET biosensors inclusive of nanomaterials growth, device fabrication, sensing mechanisms, and interaction of biomolecules with nanotubes and nanowires. Design considerations, factors affecting sensing performance and sensitivity, amplification and multiplexing strategies are also detailed to provide a comprehensive understanding of present biosensors and future sensor systems development.

Direct Detection of Heroin Metabolites Using a Competitive Immunoassay Based on a Carbon‐Nanotube Liquid‐Gated Field‐Effect Transistor

A carbon-nanotube-based liquid-gated field-effect transistor is employed for the detection of heroin narcotics. Detection of monoacetylmorphine down to 15 pg mL−1 is accomplished by means of a competitive immunoassay protocol in conjunction with charged Au nanoparticles that augment the electrostatic perturbance generated from the receptor–ligand interaction coupled with the carbon nanotubes.

Femtomolar detection of2,4-dichlorophenoxyacetic acidherbicidesvia competitive immunoassays using microfluidic based carbon nanotube liquid gated transistor

Monitoring of environmental pollutants has become increasingly important due to concern over potential health and environmental impact inflicted by these chemicals. In this contribution, we focus on the development of an all-plastic biosensor comprising laminated single-walled carbon nanotubes as the active element and its conductance modulation in a liquid-gated field effect transistor, as the principle of transduction, for the detection of 2,4-dicholorophenoxy acetic acid (2,4-D) herbicide. The reported biosensor is capable of performing real-time label-free detection of analytes in liquid environment. This biosensor which relies on immunoassay principle for specificity is able to detect down to 500 fM levels of 2,4-D in soil samples.