TY - JOUR A1 - Yoshinobu, Tatsuo A1 - Miyamoto, Ko-ichiro A1 - Werner, Frederik A1 - Poghossian, Arshak A1 - Wagner, Torsten A1 - Schöning, Michael Josef T1 - Light-addressable potentiometric sensors for quantitative spatial imaging of chemical species JF - Annual Review of Analytical Chemistry N2 - A light-addressable potentiometric sensor (LAPS) is a semiconductor-based chemical sensor, in which a measurement site on the sensing surface is defined by illumination. This light addressability can be applied to visualize the spatial distribution of pH or the concentration of a specific chemical species, with potential applications in the fields of chemistry, materials science, biology, and medicine. In this review, the features of this chemical imaging sensor technology are compared with those of other technologies. Instrumentation, principles of operation, and various measurement modes of chemical imaging sensor systems are described. The review discusses and summarizes state-of-the-art technologies, especially with regard to the spatial resolution and measurement speed; for example, a high spatial resolution in a submicron range and a readout speed in the range of several tens of thousands of pixels per second have been achieved with the LAPS. The possibility of combining this technology with microfluidic devices and other potential future developments are discussed. Y1 - 2017 U6 - http://dx.doi.org/10.1146/annurev-anchem-061516-045158 SN - 1936-1327 VL - 10 SP - 225 EP - 246 PB - Annual Reviews CY - Palo Alto, Calif. ER - TY - JOUR A1 - Werner, Frederik A1 - Miyamoto, Ko-ichiro A1 - Wagner, Torsten A1 - Schöning, Michael Josef A1 - Yoshinobu, Tatsuo T1 - Lateral resolution enhancement of pulse-driven light-addressable potentiometric sensor JF - Sensor and Actuators B: Chemical N2 - To study chemical and biological processes, spatially resolved determination of the concentrations of one or more analyte species is of distinct interest. With a light-addressable potentiometric sensor (LAPS), chemical images can be created, which visualize the concentration distribution above the sensor plate. One important challenge is to achieve a good lateral resolution in order to detect events that take place in a small and limited region. LAPS utilizes a focused light spot to address the measurement region. By moving this light spot along the semiconductor sensor plate, the concentration distribution can be observed. In this study, we show that utilizing a pulse as light excitation instead of a traditionally used continuously modulated light excitation, the lateral resolution can be improved by a factor of 6 or more. KW - Chemical images KW - LAPS KW - Light-addressable potentiometric sensor Y1 - 2017 U6 - http://dx.doi.org/10.1016/j.snb.2017.02.057 SN - 0925-4005 VL - 248 SP - 961 EP - 965 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Sousa, Marcos A. M. A1 - Siqueira, Jose R. Jr. A1 - Vercik, Andres A1 - Schöning, Michael Josef A1 - Oliveira, Osvaldo N. Jr. T1 - Determining the optimized layer-by-layer film architecture with dendrimer/carbon nanotubes for field-effect sensors JF - IEEE Sensors Journal N2 - The capacitive electrolyte–insulator–semiconductor (EIS) structure is a typical device based on a field-effect sensor platform. With a simple silicon-based structure, EIS have been useful for several sensing applications, especially with incorporation of nanostructured films to modulate the ionic transport and the flat-band potential. In this paper, we report on ion transport and changes in flat-band potential in EIS sensors made with layer-by-layer films containing poly(amidoamine) (PAMAM) dendrimer and single-walled carbon nanotubes (SWNTs) adsorbed on p-Si/SiO 2 /Ta 2 O 5 chips with an Al ohmic contact. The impedance spectra were fitted using an equivalent circuit model, from which we could determine parameters such as the double-layer capacitance. This capacitance decreased with the number of bilayers owing to space charge accumulated at the electrolyte–insulator interface, up to three PAMAM/SWNTs bilayers, after which it stabilized. The charge-transfer resistance was also minimum for three bilayers, thus indicating that this is the ideal architecture for an optimized EIS performance. The understanding of the influence of nanostructures and the fine control of operation parameters pave the way for optimizing the design and performance of new EIS sensors. Y1 - 2017 U6 - http://dx.doi.org/10.1109/JSEN.2017.2653238 SN - 1558-1748 VL - 17 IS - 6 SP - 1735 EP - 1740 PB - IEEE CY - New York ER - TY - JOUR A1 - Schöning, Michael Josef A1 - Bronder, Thomas A1 - Wu, Chunsheng A1 - Scheja, Sabrina A1 - Jessing, Max A1 - Metzger-Boddien, Christoph A1 - Keusgen, Michael A1 - Poghossian, Arshak T1 - Label-Free DNA Detection with Capacitive Field-Effect Devices—Challenges and Opportunities JF - Proceedings N2 - Field-effect EIS (electrolyte-insulator-semiconductor) sensors modified with a positively charged weak polyelectrolyte layer have been applied for the electrical detection of DNA (deoxyribonucleic acid) immobilization and hybridization by the intrinsic molecular charge. The EIS sensors are able to detect the existence of target DNA amplicons in PCR (polymerase chain reaction) samples and thus, can be used as tool for a quick verification of DNA amplification and the successful PCR process. Due to their miniaturized setup, compatibility with advanced micro- and nanotechnologies, and ability to detect biomolecules by their intrinsic molecular charge, those sensors can serve as possible platform for the development of label-free DNA chips. Possible application fields as well as challenges and limitations will be discussed. Y1 - 2017 U6 - http://dx.doi.org/10.3390/proceedings1080719 SN - 2504-3900 N1 - This article belongs to the Proceedings of "Proceedings of the 5th International Symposium on Sensor Science (I3S 2017)" VL - 1 IS - 8 SP - Artikel 719 PB - MDPI CY - Basel ER - TY - JOUR A1 - Scholl, Fabio A1 - Morais, Paulo A1 - Gabriel, Rayla A1 - Schöning, Michael Josef A1 - Siqueira, Jose Roberto, Jr. A1 - Caseli, Luciano T1 - Carbon nanotubes arranged as smart interfaces in lipid Langmuir-Blodgett films enhancing the enzymatic properties of penicillinase for biosensing applications JF - Applied Materials & Interfaces N2 - In this paper, carbon nanotubes (CNTs) were incorporated in penicillinase-phospholipid Langmuir and Langmuir–Blodgett (LB) films to enhance the enzyme catalytic properties. Adsorption of the penicillinase and CNTs at dimyristoylphosphatidic acid (DMPA) monolayers at the air–water interface was investigated by surface pressure–area isotherms, vibrational spectroscopy, and Brewster angle microscopy. The floating monolayers were transferred to solid supports through the LB technique, forming mixed DMPA-CNTs-PEN films, which were investigated by quartz crystal microbalance, vibrational spectroscopy, and atomic force microscopy. Enzyme activity was studied with UV–vis spectroscopy and the feasibility of the supramolecular device nanostructured as ultrathin films were essayed in a capacitive electrolyte–insulator–semiconductor (EIS) sensor device. The presence of CNTs in the enzyme–lipid LB film not only tuned the catalytic activity of penicillinase but also helped conserve its enzyme activity after weeks, showing increased values of activity. Viability as penicillin sensor was demonstrated with capacitance/voltage and constant capacitance measurements, exhibiting regular and distinctive output signals over all concentrations used in this work. These results may be related not only to the nanostructured system provided by the film, but also to the synergism between the compounds on the active layer, leading to a surface morphology that allowed a fast analyte diffusion because of an adequate molecular accommodation, which also preserved the penicillinase activity. This work therefore demonstrates the feasibility of employing LB films composed of lipids, CNTs, and enzymes as EIS devices for biosensing applications. Y1 - 2017 U6 - http://dx.doi.org/10.1021/acsami.7b08095 SN - 1944-8252 VL - 9 IS - 36 SP - 31054 EP - 31066 PB - ACS CY - Washington ER - TY - JOUR A1 - Röhlen, Desiree A1 - Pilas, Johanna A1 - Schöning, Michael Josef A1 - Selmer, Thorsten T1 - Development of an amperometric biosensor platform for the combined determination of l-Malic, Fumaric, and l-Aspartic acid JF - Applied Biochemistry and Biotechnology N2 - Three amperometric biosensors have been developed for the detection of L-malic acid, fumaric acid, and L -aspartic acid, all based on the combination of a malate-specific dehydrogenase (MDH, EC 1.1.1.37) and diaphorase (DIA, EC 1.8.1.4). The stepwise expansion of the malate platform with the enzymes fumarate hydratase (FH, EC 4.2.1.2) and aspartate ammonia-lyase (ASPA, EC 4.3.1.1) resulted in multi-enzyme reaction cascades and, thus, augmentation of the substrate spectrum of the sensors. Electrochemical measurements were carried out in presence of the cofactor β-nicotinamide adenine dinucleotide (NAD+) and the redox mediator hexacyanoferrate (III) (HCFIII). The amperometric detection is mediated by oxidation of hexacyanoferrate (II) (HCFII) at an applied potential of + 0.3 V vs. Ag/AgCl. For each biosensor, optimum working conditions were defined by adjustment of cofactor concentrations, buffer pH, and immobilization procedure. Under these improved conditions, amperometric responses were linear up to 3.0 mM for L-malate and fumarate, respectively, with a corresponding sensitivity of 0.7 μA mM−1 (L-malate biosensor) and 0.4 μA mM−1 (fumarate biosensor). The L-aspartate detection system displayed a linear range of 1.0–10.0 mM with a sensitivity of 0.09 μA mM−1. The sensor characteristics suggest that the developed platform provides a promising method for the detection and differentiation of the three substrates. Y1 - 2017 U6 - http://dx.doi.org/10.1007/s12010-017-2578-1 SN - 1559-0291 VL - 183 SP - 566 EP - 581 PB - Springer CY - Berlin ER - TY - JOUR A1 - Poghossian, Arshak A1 - Werner, Frederik A1 - Buniatyan, V. V. A1 - Wagner, Torsten A1 - Miamoto, K. A1 - Yoshinobu, T. A1 - Schöning, Michael Josef T1 - Towards addressability of light-addressable potentiometric sensors: Shunting effect of non-illuminated region and cross-talk JF - Sensor and Actuators B: Chemical N2 - The LAPS (light-addressable potentiometric sensor) platform is one of the most attractive approaches for chemical and biological sensing with many applications ranging from pH and ion/analyte concentration measurements up to cell metabolism detection and chemical imaging. However, although it is generally accepted that LAPS measurements are spatially resolved, the light-addressability feature of LAPS devices has not been discussed in detail so far. In this work, an extended electrical equivalent-circuit model of the LAPS has been presented, which takes into account possible cross-talk effects due to the capacitive coupling of the non-illuminated region. A shunting effect of the non-illuminated area on the measured photocurrent and addressability of LAPS devices has been studied. It has been shown, that the measured photocurrent will be determined not only by the local interfacial potential in the illuminated region but also by possible interfacial potential changes in the non-illuminated region, yielding cross-talk effects. These findings were supported by the experimental investigations of a penicillin-sensitive multi-spot LAPS and a metal-insulator-semiconductor LAPS as model systems. Y1 - 2017 U6 - http://dx.doi.org/10.1016/j.snb.2017.01.047 SN - 0925-4005 IS - 244 SP - 1071 EP - 1079 PB - Elsevier CY - Amsterdam ER - TY - CHAP A1 - Poghossian, Arshak A1 - Schöning, Michael Josef T1 - Nanomaterial-Modified Capacitive Field-Effect Biosensors T2 - Springer Series on Chemical Sensors and Biosensors (Methods and Applications) N2 - The coupling of charged molecules, nanoparticles, and more generally, inorganic/organic nanohybrids with semiconductor field-effect devices based on an electrolyte–insulator–semiconductor (EIS) system represents a very promising strategy for the active tuning of electrochemical properties of these devices and, thus, opening new opportunities for label-free biosensing by the intrinsic charge of molecules. The simplest field-effect sensor is a capacitive EIS sensor, which represents a (bio-)chemically sensitive capacitor. In this chapter, selected examples of recent developments in the field of label-free biosensing using nanomaterial-modified capacitive EIS sensors are summarized. In the first part, we present applications of EIS sensors modified with negatively charged gold nanoparticles for the label-free electrostatic detection of positively charged small proteins and macromolecules, for monitoring the layer-by-layer formation of oppositely charged polyelectrolyte (PE) multilayers as well as for the development of an enzyme-based biomolecular logic gate. In the second part, examples of a label-free detection by means of EIS sensors modified with a positively charged weak PE layer are demonstrated. These include electrical detection of on-chip and in-solution hybridized DNA (deoxyribonucleic acid) as well as an EIS sensor with pH-responsive weak PE/enzyme multilayers for enhanced field-effect biosensing. KW - Biomolecular logic gate KW - DNA KW - Enzyme biosensor KW - Field-effect sensor KW - Gold nanoparticle Y1 - 2017 U6 - http://dx.doi.org/10.1007/5346_2017_2 SP - 1 EP - 25 PB - Springer CY - Berlin, Heidelberg ER - TY - JOUR A1 - Pilas, Johanna A1 - Yazici, Yasemen A1 - Selmer, Thorsten A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Optimization of an amperometric biosensor array for simultaneous measurement of ethanol, formate, d- and l-lactate JF - Electrochimica Acta N2 - The immobilization of NAD+-dependent dehydrogenases, in combination with a diaphorase, enables the facile development of multiparametric sensing devices. In this work, an amperometric biosensor array for simultaneous determination of ethanol, formate, d- and l-lactate is presented. Enzyme immobilization on platinum thin-film electrodes was realized by chemical cross-linking with glutaraldehyde. The optimization of the sensor performance was investigated with regard to enzyme loading, glutaraldehyde concentration, pH, cofactor concentration and temperature. Under optimal working conditions (potassium phosphate buffer with pH 7.5, 2.5 mmol L-1 NAD+, 2.0 mmol L-1 ferricyanide, 25 °C and 0.4% glutaraldehyde) the linear working range and sensitivity of the four sensor elements was improved. Simultaneous and cross-talk free measurements of four different metabolic parameters were performed successfully. The reliable analytical performance of the biosensor array was demonstrated by application in a clarified sample of inoculum sludge. Thereby, a promising approach for on-site monitoring of fermentation processes is provided. KW - Simultaneous determination KW - Enzymatic biosensor KW - Diaphorase KW - Dehydrogenase Y1 - 2017 U6 - http://dx.doi.org/10.1016/j.electacta.2017.07.119 SN - 0013-4686 VL - 251 SP - 256 EP - 262 PB - Elsevier CY - Amsterdam ER - TY - CHAP A1 - Oberländer, Jan A1 - Arreola, Julio A1 - Hansen, Christina A1 - Greeff, Anton A1 - Mayer, Marlena A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Impedimetric Biosensor to Enable Fast Evaluation of Gaseous Sterilization Processes T2 - MDPI Proceedings Y1 - 2017 U6 - http://dx.doi.org/10.3390/proceedings1040435 N1 - Eurosensors 2017 Conference, Paris, France, 3–6 September 2017 VL - 1 IS - 4 ER -