Recent Developments of High-Resolution Chemical Imaging Systems Based on Light-Addressable Potentiometric Sensors (LAPSs).
ABSTRACT: A light-addressable potentiometric sensor (LAPS) is a semiconductor electrochemical sensor based on the field-effect which detects the variation of the Nernst potential on the sensor surface, and the measurement area is defined by illumination. Thanks to its light-addressability feature, an LAPS-based chemical imaging sensor system can be developed, which can visualize the two-dimensional distribution of chemical species on the sensor surface. This sensor system has been used for the analysis of reactions and diffusions in various biochemical samples. In this review, the LAPS system set-up, including the sensor construction, sensing and substrate materials, modulated light and various measurement modes of the sensor systems are described. The recently developed technologies and the affecting factors, especially regarding the spatial resolution and temporal resolution are discussed and summarized, and the advantages and limitations of these technologies are illustrated. Finally, the further applications of LAPS-based chemical imaging sensors are discussed, where the combination with microfluidic devices is promising.
Project description:The sensing mechanism of binding Hg(2+) into thymine-thymine (T-T) mismatched base pairs was introduced into a light-addressable potentiometric sensor (LAPS) with anti-Hg(2+) aptamer as the sensing units. Three kinds of T-rich single-strand DNA (ssDNA) chains with different spacer lengths, from 0 to 12 -CH? groups, were designed to investigate surface charge and morphological effects on the LAPS' output. First, by comparing the responding of LAPS modified with three kinds of ssDNA, it was found that the best performance for Hg(2+) sensing was exhibited by the probe without -CH? groups. The detection limit of Hg(2+) ion was 1 ppt under the optimal condition. Second, the cooperative effects of surface charge and morphology on the output were observed by the controlled experiments. The two effects were the negative charge balanced by metal cations and the morphological changing caused by the formation of T-Hg(2+)-T structure. In conclusion, not only the influences of the aptamer probe's morphology and surface charge was investigated on the platform of LAPS, but also sensing Hg(2+) ions was achieved for the first time by the presented aptamer LAPS.
Project description:DNA methylation (DNAm) sensors are an emerging branch in the discipline of sensors. It is believed to be able to promote the next generation of epigenetics-based diagnostic technology. Differing from the traditional biochemical sensors that aimed at individual molecules, the challenge in DNAm sensors is how to determine the amount of 5-methylcytosine (5mC) in a continuous nucleotide sequence. Here, we report a comparative study about meso-tetra(4-carboxyphenyl)porphine (TCPP)-based DNAm sensing interfaces on a light-addressable potentiometric sensor (LAPS), depending on TCPP's postures that are flat in the ?-conjugated TCPP layer on reduced-graphene-oxide-decorated LAPS (#1) and stand-up in the covalently anchored TCPP on glutaraldehyde (GA)-treated LAPS (#2), along with the blank one (only GA-treated LAPS, #3). These DNAm sensing interfaces are also distinct from the traditional biosensing interface on LAPS, that is: it is not functionalized by the sensing indicator (5mC antibody, in this case) but by the target nucleotide sequence. The surface characterization techniques such as Raman spectra, scanning electron microscopy, and X-ray photoelectron spectroscopy are conducted to prove the decorations, as well as the anchored nucleotides. It is found that, though all of them can detect as low as one 5mC in the target sequence, the enhanced DNAm sensitivity is obtained by #2, which is evidenced by the higher output-voltage changing ratio for the 5mC site of #2 than those of #1 and #3. Furthermore, the underlying causes for the improved sensitivity in #2 are proposed, according to the conformational and electronic properties of TCPP molecules. Conclusively, TCPP's synergetic function, including the molecular configuration and the activate (carboxyl) groups on its peripheral substituents, to improve the DNAm sensing interface on LAPS is investigated and demonstrated. This can shed light on a new approach for DNA methylation detection, with the merits of low cost, independence on bisulfite conversion, and polymerase chain reaction.
Project description:Potentiometric transduction is an important tool of analytical chemistry to record chemical signals, but some constraints in the miniaturization and low-cost fabrication of the reference electrode are a bottleneck in the realization of more-advanced devices such as wearable and lab-on-a-chip sensors. Here, an organic electrochemical transistor (OECT) has been designed with an alternative architecture that allows to record the potentiometric signals of gate electrodes, which have been chemically modified to obtain Ag/AgnX interfaces (X = Cl-, Br-, I-, and S2-), without the use of a reference electrode. When the OECT is immersed in a sample solution, it reaches an equilibrium state, because PEDOT:PSS exchanges charges with the electrolyte until its Fermi level is aligned to the one of Ag/AgnX. The latter is controlled by Xn- concentration in the solution. As a consequence, in this spontaneous process, the conductivity of PEDOT:PSS changes with the electrochemical potential of the modified gate electrode without any external bias. The sensor works by applying only a fixed drain current or drain voltage and thus the OECT sensor operates with just two terminals. It is also demonstrated that, in this configuration, gate potential values extracted from the drain current are in good agreement with the ones measured with respect to a reference electrode being perfectly correlated (linear slope equal to 1.00 ± 0.03). In the case of the sulfide anion, the OECT performance overcomes the limit represented by the Nernst equation, with a sensitivity of 0.52 V decade-1. The presented results suggest that OECTs could be a viable option to fabricate advanced sensors based on potentiometric transduction.
Project description:Phosphorus donor impurities in silicon are a promising candidate for solid-state quantum computing due to their exceptionally long coherence times and high fidelities. However, individual addressability of exchange coupled donors with separations ~15 nm is challenging. We show that by using atomic precision lithography, we can place a single P donor next to a 2P molecule 16 ± 1 nm apart and use their distinctive hyperfine coupling strengths to address qubits at vastly different resonance frequencies. In particular, the single donor yields two hyperfine peaks separated by 97 ± 2.5 MHz, in contrast to the donor molecule that exhibits three peaks separated by 262 ± 10 MHz. Atomistic tight-binding simulations confirm the large hyperfine interaction strength in the 2P molecule with an interdonor separation of ~0.7 nm, consistent with lithographic scanning tunneling microscopy images of the 2P site during device fabrication. We discuss the viability of using donor molecules for built-in addressability of electron spin qubits in silicon.
Project description:We report a new hybrid integration scheme that offers for the first time a nanowire-on-lead approach, which enables independent electrical addressability, is scalable, and has superior spatial resolution in vertical nanowire arrays. The fabrication of these nanowire arrays is demonstrated to be scalable down to submicrometer site-to-site spacing and can be combined with standard integrated circuit fabrication technologies. We utilize these arrays to perform electrophysiological recordings from mouse and rat primary neurons and human induced pluripotent stem cell (hiPSC)-derived neurons, which revealed high signal-to-noise ratios and sensitivity to subthreshold postsynaptic potentials (PSPs). We measured electrical activity from rodent neurons from 8 days in vitro (DIV) to 14 DIV and from hiPSC-derived neurons at 6 weeks in vitro post culture with signal amplitudes up to 99 mV. Overall, our platform paves the way for longitudinal electrophysiological experiments on synaptic activity in human iPSC based disease models of neuronal networks, critical for understanding the mechanisms of neurological diseases and for developing drugs to treat them.
Project description:Monitoring the cellular metabolism of bacteria in (bio)fermentation processes is crucial to control and steer them, and to prevent undesired disturbances linked to metabolically inactive microorganisms. In this context, cell-based biosensors can play an important role to improve the quality and increase the yield of such processes. This work describes the simultaneous analysis of the metabolic behavior of three different types of bacteria by means of a differential light-addressable potentiometric sensor (LAPS) set-up. The study includes Lactobacillus brevis, Corynebacterium glutamicum, and Escherichia coli, which are often applied in fermentation processes in bioreactors. Differential measurements were carried out to compensate undesirable influences such as sensor signal drift, and pH value variation during the measurements. Furthermore, calibration curves of the cellular metabolism were established as a function of the glucose concentration or cell number variation with all three model microorganisms. In this context, simultaneous (bio)sensing with the multi-organism LAPS-based set-up can open new possibilities for a cost-effective, rapid detection of the extracellular acidification of bacteria on a single sensor chip. It can be applied to evaluate the metabolic response of bacteria populations in a (bio)fermentation process, for instance, in the biogas fermentation process.
Project description:The Field Effect sensors are broadly used for detecting various target analytes in chemical and biological solutions. We report the conditions under which the pH sensitivity of an Ion Sensitive Field Effect transistor (ISFET) sensor can be significantly enhanced. Our theory and simulations show that by using pH buffer solutions containing counter-ions that are beyond a specific size, the sensor shows significantly higher sensitivity which can exceed the Nernst limit. We validate the theory by measuring the pH response of an extended gate ISFET pH sensor. The consistency and reproducibility of the measurement results have been recorded in hysteresis free and stable operations. Different conditions have been tested to confirm the accuracy and validity of our experiment results such as using different solutions, various oxide dielectrics as the sensing layer and off-the-shelf versus IC fabricated transistors as the basis of the ISFET sensor.
Project description:Advances in the miniaturization and portability of the chemical sensing devices have always been hindered by the external power supply problem, which has focused new interest in the fabrication of self-powered sensing devices for disease diagnosis and the monitoring of analytes. This review describes the fabrication of ZnO nanomaterial-based sensors synthesized on different conducting substrates for extracellular detection, and the use of a sharp borosilicate glass capillary (diameter, d = 700 nm) to grow ZnO nanostructures for intracellular detection purposes in individual human and frog cells. The electrocatalytic activity and fast electron transfer properties of the ZnO materials provide the necessary energy to operate as well as a quick sensing device output response, where the role of the nanomorphology utilized for the fabrication of the sensor is crucial for the production of the operational energy. Simplicity, design, cost, sensitivity, selectivity and a quick and stable response are the most important features of a reliable sensor for routine applications. The review details the extra- and intra-cellular applications of the biosensors for the detection and monitoring of different metallic ions present in biological matrices, along with the biomolecules glucose and cholesterol.
Project description:Gas exhaust emissions in vehicles are increasingly restrictive in EU and USA. Diesel engines are particularly affected by limitation in hydrocarbons and NOx concentrations. This work presents a screening of working electrode materials to develop a potentiometric sensor, with the most promising material to detect being C?H? at 550 °C. The device consists of a dense 8YSZ (8 mol% Y?O? stabilized ZrO?) disk as oxide-ion conducting electrolyte, whereas platinum is screen-printed in the back face as reference electrode. As working electrode, several materials such as Fe0.7Cr1.3O?, ZnCr?O?, Fe?NiO?, La0.8Sr0.2CrO3-? (LSC), La0.8Sr0.2MnO? (LSM), and NiO+5%wt Au were tested to detect C?H?. Sensor voltage was measured for several concentrations of C?H? and CO as these are two of the major oxidizable compounds in a diesel exhaust gas. Fe0.7Cr1.3O? was selected as the most promising material because of its response to C?H? and CO. Not only is the response to the individual analytes important, but the C?H? cross-sensitivity toward CO is also important. Fe0.7Cr1.3O? showed a good performance to C?H?, with low cross-sensitivity to CO. In addition, when 0.16 ppm of phenanthrene is added, the sensor still has a slightly better response to C?H? than to CO. Nevertheless, the sensor exposure to high concentrations (>85 ppm) of polycyclic aromatic hydrocarbons led to signal saturation. On the other hand, the operation in wet conditions induces lower sensor sensitivity to C?H? and higher cross-sensitivity toward CO increase, i.e., the sensor response becomes similar for C?H? and CO.
Project description:In this work, we present a potentiometric pH sensor on textile substrate for wearable applications. The sensitive (thick film graphite composite) and reference electrodes (Ag/AgCl) are printed on cellulose-polyester blend cloth. An excellent adhesion between printed electrodes allow the textile-based sensor to be washed with a reliable pH response. The developed textile-based pH sensor works on the basis of electrochemical reaction, as observed through the potentiometric, cyclic voltammetry (100 mV/s) and electrochemical impedance spectroscopic (10 mHz to 1 MHz) analysis. The electrochemical double layer formation and the ionic exchanges of the sensitive electrode-pH solution interaction are observed through the electrochemical impedance spectroscopic analysis. Potentiometric analysis reveals that the fabricated textile-based sensor exhibits a sensitivity (slope factor) of 4 mV/pH with a response time of 5 s in the pH range 6⁻9. The presented sensor shows stable response with a potential of 47 ± 2 mV for long time (2000 s) even after it was washed in tap water. These results indicate that the sensor can be used for wearable applications.