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Light-addressable potentiometric sensors for quantitative spatial imaging of chemical species
(2017)
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.
This work describes the novel combination of the light-addressable electrode (LAE) and the light-addressable potentiometric sensor (LAPS) into a microsystem set-up. Both the LAE as well as the LAPS shares the principle of addressing the active spot by means of a light beam. This enables both systems to manipulate resp. to detect an analyte with a high spatial resolution. Hence, combining both principles into a single set-up enables the active stimulation e.g., by means of electrolysis and a simultaneous observation e.g., the response of an entrapped biological cell by detection of extracellular pH changes. The work will describe the principles of both technologies and the necessary steps to integrate them into a single set-up. Furthermore, examples of application and operation of such systems will be presented.
Light-addressable potentiometric sensor as a sensing element in plug-based microfluidic devices
(2016)
A plug-based microfluidic system based on the principle of the light-addressable potentiometric sensor (LAPS) is proposed. The LAPS is a semiconductor-based chemical sensor, which has a free addressability of the measurement point on the sensing surface. By combining a microfluidic device and LAPS, ion sensing can be performed anywhere inside the microfluidic channel. In this study, the sample solution to be measured was introduced into the channel in a form of a plug with a volume in the range of microliters. Taking advantage of the light-addressability, the position of the plug could be monitored and pneumatically controlled. With the developed system, the pH value of a plug with a volume down to 400 nL could be measured. As an example of plug-based operation, two plugs were merged in the channel, and the pH change was detected by differential measurement.
LAPS are field-effect-based potentiometric sensors which are able to monitor analyte concentrations in a spatially resolved manner. Hence, a LAPS sensor system is a powerful device to record chemical imaging of the concentration of chemical species in an aqueous solution, chemical reactions, or the growth of cell colonies on the sensor surface, to record chemical images. In this work, multi-chamber 3D-printed structures made out of polymer (PP-ABS) were combined with LAPS chips to analyse differentially and simultaneously the metabolic activity of Escherichia coli K12 and Chinese hamster ovary (CHO) cells, and the responds of those cells to the addition of glucose solution.
The light-addressable potentiometric sensor (LAPS) has the unique feature to address different regions of a sensor surface without the need of complex structures. Measurements at different locations on the sensor surface can be performed in a common analyte solution, which distinctly simplifies the fluidic set-up. However, the measurement in a single analyte chamber prevents the application of different drugs or different concentrations of a drug to each measurement spot at the same time as in the case of multi-reservoir-based set-ups. In this work, the authors designed a LAPS-based set-up for cell culture screening that utilises magnetic beads loaded with the endotoxin (lipopolysaccharides, LPS), to generate a spatially distributed gradient of analyte concentration. Different external magnetic fields can be adjusted to move the magnetic beads loaded with a specific drug within the measurement cell. By recording the metabolic activities of a cell layer cultured on top of the LAPS surface, this work shows the possibility to apply different concentrations of a sample along the LAPS measurement spots within a common analyte solution.
In this review article, we are going to present an overview on possible applications of light-addressable electrodes (LAE) as actuator/manipulation devices besides classical electrode structures. For LAEs, the electrode material consists of a semiconductor. Illumination with a light source with the appropiate wavelength leads to the generation of electron-hole pairs which can be utilized for further photoelectrochemical reaction. Due to recent progress in light-projection technologies, highly dynamic and flexible illumination patterns can be generated, opening new possibilities for light-addressable electrodes. A short introduction on semiconductor–electrolyte interfaces with light stimulation is given together with electrode-design approaches. Towards applications, the stimulation of cells with different electrode materials and fabrication designs is explained, followed by analyte-manipulation strategies and spatially resolved photoelectrochemical deposition of different material types.
The mechanical behavior of the large intestine beyond the ultimate stress has never been investigated. Stretching beyond the ultimate stress may drastically impair the tissue microstructure, which consequently weakens its healthy state functions of absorption, temporary storage, and transportation for defecation. Due to closely similar microstructure and function with humans, biaxial tensile experiments on the porcine large intestine have been performed in this study. In this paper, we report hyperelastic characterization of the large intestine based on experiments in 102 specimens. We also report the theoretical analysis of the experimental results, including an exponential damage evolution function. The fracture energies and the threshold stresses are set as damage material parameters for the longitudinal muscular, the circumferential muscular and the submucosal collagenous layers. A biaxial tensile simulation of a linear brick element has been performed to validate the applicability of the estimated material parameters. The model successfully simulates the biomechanical response of the large intestine under physiological and non-physiological loads.
Lead and nickel, as heavy metals, are still used in industrial processes, and are classified as “environmental health hazards” due to their toxicity and polluting potential. The detection of heavy metals can prevent environmental pollution at toxic levels that are critical to human health. In this sense, the electrolyte–insulator–semiconductor (EIS) field-effect sensor is an attractive sensing platform concerning the fabrication of reusable and robust sensors to detect such substances. This study is aimed to fabricate a sensing unit on an EIS device based on Sn₃O₄ nanobelts embedded in a polyelectrolyte matrix of polyvinylpyrrolidone (PVP) and polyacrylic acid (PAA) using the layer-by-layer (LbL) technique. The EIS-Sn₃O₄ sensor exhibited enhanced electrochemical performance for detecting Pb²⁺ and Ni²⁺ ions, revealing a higher affinity for Pb²⁺ ions, with sensitivities of ca. 25.8 mV/decade and 2.4 mV/decade, respectively. Such results indicate that Sn₃O₄ nanobelts can contemplate a feasible proof-of-concept capacitive field-effect sensor for heavy metal detection, envisaging other future studies focusing on environmental monitoring.
Layer-by-Layer Assembly of Carbon Nanotubes Incorporated in Light-Addressable Potentiometric Sensors
(2009)
Rationale: Previous studies [Topolnik et al., Cereb Cortex 2003; 13: 883; Schindler et al., Brain 2007; 130: 65] indicate that the termination of focal onset seizures may be causally related to an increase of global neuronal correlation during the second half of the seizures. This increase was observed to occur earlier in complex partial seizures than in secondarily generalized seizures. We here address the question whether such an increase of neuronal correlation prior to seizure end is indeed a global phenomenon, involving both hemispheres or whether there are side-specific differences. Methods: We analyzed 20 focal onset seizures (10 complex partial, 10 secondarily generalized seizures) recorded in 13 patients who underwent presurgical evaluation of focal epilepsies of different origin. EEG was recorded intracranially from bilaterally implanted subdural strip and intrahippocampal depth electrodes. Utilizing a moving window approach, we investigated the evolution of the maximum cross correlation for all channel combinations during seizures. For each moving window the mean value of the maximum cross correlation (MCC) between all electrode contacts was computed separately for each hemisphere. After normalization of seizure durations, MCC values of the ipsi- and contralateral hemisphere for all seizures were determined. Results: We observed that the MCC of the contralateral hemisphere in complex partial seizures increased during the first half of the seizure, whereas, for the same time interval, the MCC of the ipsilateral hemisphere even declined below the level of the pre-seizure period. In contrast, no significant differences between both hemispheres could be observed for secondarily generalized seizures where both hemispheres showed a simultaneous increase of MCC during the second half of the seizures. The level of MCC for the contralateral hemisphere was higher for complex partial seizures than for secondarily generalized seizures during the first half of the seizure. Conclusions: Our findings indicate that there are indeed lateralized differences in the evolution of global neuronal correlation during complex partial and secondarily generalized seizures. The observed contralateral increase of neuronal correlation during complex partial seizures might indicate an emerging self-organizing mechanism for preventing the spread of seizure activity.
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.
LAPS-based monitoring of metabolic responses of bacterial cultures in a paper fermentation broth
(2020)
As an alternative renewable energy source, methane production in biogas plants is gaining more and more attention. Biomass in a bioreactor contains different types of microorganisms, which should be considered in terms of process-stability control. Metabolically inactive microorganisms within the fermentation process can lead to undesirable, time-consuming and cost-intensive interventions. Hence, monitoring of the cellular metabolism of bacterial populations in a fermentation broth is crucial to improve the biogas production, operation efficiency, and sustainability. In this work, the extracellular acidification of bacteria in a paper-fermentation broth is monitored after glucose uptake, utilizing a differential light-addressable potentiometric sensor (LAPS) system. The LAPS system is loaded with three different model microorganisms (Escherichia coli, Corynebacterium glutamicum, and Lactobacillus brevis) and the effect of the fermentation broth at different process stages on the metabolism of these bacteria is studied. In this way, different signal patterns related to the metabolic response of microorganisms can be identified. By means of calibration curves after glucose uptake, the overall extracellular acidification of bacterial populations within the fermentation process can be evaluated.
Among the variety of transducer concepts proposed for label-free detection of biomolecules, the semiconductor field-effect device (FED) is one of the most attractive platforms. As medical techniques continue to progress towards diagnostic and therapies based on biomarkers, the ability of FEDs for a label-free, fast and real-time detection of multiple pathogenic and physiologically relevant molecules with high specificity and sensitivity offers very promising prospects for their application in point-of-care and personalized medicine for an early diagnosis and treatment of diseases. The presented paper reviews recent advances and current trends in research and development of different FEDs for label-free, direct electrical detection of charged biomolecules by their intrinsic molecular charge. The authors are mainly focusing on the detection of the DNA hybridization event, antibody-antigen affinity reaction as well as clinically relevant biomolecules such as cardiac and cancer biomarkers.
Label-free sensing of biomolecules by their intrinsic molecular charge using field-effect devices
(2015)
Label-free Electrostatic Detection of DNA Amplification by PCR Using Capacitive Field-effect Devices
(2016)
A capacitive field-effect EIS (electrolyte-insulator-semiconductor) sensor modified with a positively charged weak polyelectrolyte of poly(allylamine hydrochloride) (PAH)/single-stranded probe DNA (ssDNA) bilayer has been used for a label-free electrostatic detection of pathogen-specific DNA amplification via polymerase chain reaction (PCR). The sensor is able to distinguish between positive and negative PCR solutions, to detect the existence of target DNA amplicons in PCR samples and thus, can be used as tool for a quick verification of DNA amplification and the successful PCR process.
A multi-spot (4 × 4 spots) light-addressable potentiometric sensor (MLAPS) consisting of an Al–p-Si–SiO2 structure has been applied for the label-free electrical detection of DNA (deoxyribonucleic acid) immobilization and hybridization by the intrinsic molecular charge for the first time. Single-stranded probe ssDNA molecules (20 bases) were covalently immobilized onto the silanized SiO2 gate surface. The unspecific adsorption of mismatch ssDNA on the MLAPS gate surface was blocked by bovine serum albumin molecules. To reduce the screening effect and to achieve a high sensor signal, the measurements were performed in a low ionic-strength solution. The photocurrent–voltage (I–V) curves were simultaneously recorded on all 16 spots after each surface functionalization step. Large shifts of I–V curves of 25 mV were registered after the DNA immobilization and hybridization event. In contrast, a small potential shift (∼5 mV) was observed in case of mismatch ssDNA, revealing good specificity of the sensor. The obtained results demonstrate the potential of the MLAPS as promising transducer platform for the multi-spot label-free electrical detection of DNA molecules by their intrinsic molecular charge.
Label-free electrical detection of consecutive deoxyribonucleic acid (DNA) hybridization/denaturation by means of an array of individually addressable field-effect-based nanoplate silicon-on-insulator (SOI) capacitors modified with gold nanoparticles (Au-NP) is investigated. The proposed device detects charge changes on Au-NP/DNA hybrids induced by the hybridization or denaturation event. DNA hybridization was performed in a high ionic-strength solution to provide a high hybridization efficiency. On the other hand, to reduce the screening of the DNA charge by counter ions and to achieve a high sensitivity, the sensor signal induced by the hybridization and denaturation events was measured in a low ionic-strength solution. High sensor signals of about 120, 90, and 80 mV were registered after the DNA hybridization, denaturation, and re-hybridization events, respectively. Fluorescence microscopy has been applied as reference method to verify the DNA immobilization, hybridization, and denaturation processes. An electrostatic charge-plane model for potential changes at the gate surface of a nanoplate field-effect sensor induced by the DNA hybridization has been developed taking into account both the Debye length and the distance of the DNA charge from the gate surface.
A new approach for a label-free electrical detection of DNA hybridization and denaturation using an array of individually addressable field-effect nanoplate SOI (silicon-on-insulator) capacitors functionalized with gold nanoparticles is presented. By using a constant-capacitance measuring setup in a differential mode, signal changes of ∼110 mV and ∼70 mV have been registered after the DNA hybridization and denaturation events, respectively.
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.
In this study, polyelectrolyte-modified field-effect-based electrolyte-insulator-semiconductor (EIS) devices have been used for the label-free electrical detection of double-stranded deoxyribonucleic acid (dsDNA)molecules. The sensor-chip functionalization with a positively charged polyelectrolyte layer provides the possibility of direct adsorptive binding of negatively charged target DNA oligonucleotides onto theSiO2-chip surface.EIS sensors can be utilized as a tool to detect surface-charge changes; the electrostatic adsorption of oligonucleotides onto the polyelectrolyte layer leads to a measureable surface-potential change. Signals of 39mV have been recorded after the incubation with the oligonucleotide solution. Besides the electrochemical experiments, the successful adsorption of dsDNA onto the polyelectrolyte layer has been verified via fluorescence microscopy. The presented results demonstrate that the signal recording of EISchips, which are modified with a polyelectrolyte layer, canbe used as a favorable approach for a fast, cheap and simple detection method for dsDNA.
A multi-spot (16 spots) light-addressable potentiometric sensor (MLAPS) consisting of an Al–p-Si–SiO2 structure modified with a weak polyelectrolyte layer of PAH (poly(allylamine hydrochloride)) was applied for the label-free electrical detection of DNA (deoxyribonucleic acid) immobilization and hybridization by the intrinsic molecular charge for the first time. To achieve a preferentially flat orientation of DNA strands and thus, to reduce the distance between the DNA charge and MLAPS surface, the negatively charged probe single-stranded DNAs (ssDNA) were electrostatically adsorbed onto the positively charged PAH layer using a simple layer-by-layer (LbL) technique. In this way, more DNA charge can be positioned within the Debye length, yielding a higher sensor signal. The surface potential changes in each spot induced due to the surface modification steps (PAH adsorption, probe ssDNA immobilization, hybridization with complementary target DNA (cDNA), non-specific adsorption of mismatched ssDNA) were determined from the shifts of photocurrent–voltage curves along the voltage axis. A high sensor signal of 83 mV was registered after immobilization of probe ssDNA onto the PAH layer. The hybridization signal increases from 5 mV to 32 mV with increasing the concentration of cDNA from 0.1 nM to 5 μM. In contrast, a small signal of 5 mV was recorded in the case of non-specific adsorption of fully mismatched ssDNA (5 μM). The obtained results demonstrate the potential of the MLAPS in combination with the simple and rapid LbL immobilization technique as a promising platform for the future development of multi-spot light-addressable label-free DNA chips with direct electrical readout.
Light-addressable potentiometric sensors (LAPS) consisting of a p-Si-SiO2 and p-Si-SiO2-Au structure, respectively, have been tested for a label-free electrical detection of DNA (deoxyribonucleic acid) hybridization. Three different strategies for immobilizing single-stranded probe DNA (ssDNA) molecules on a LAPS surface have been studied and compared: (a) immobilization of thiol-modified ssDNA on the patterned Au surface via gold-thiol bond, (b) covalent immobilization of amino-modified ssDNA onto the SiO2 surface functionalized with 3-aminopropyltriethoxysilane and (c) layer-by-layer adsorption of negatively charged ssDNA on a positively charged weak polyelectrolyte layer of poly(allylamine hydrochloride).
Kyphoplasty of Osteoporotic Fractured Vertebrae: A Finite Element Analysis about Two Types of Cement
(2019)
Due to the transition to renewable energies, electricity markets need to be made fit for purpose. To enable the comparison of different energy market designs, modeling tools covering market actors and their heterogeneous behavior are needed. Agent-based models are ideally suited for this task. Such models can be used to simulate and analyze changes to market design or market mechanisms and their impact on market dynamics. In this paper, we conduct an evaluation and comparison of two actively developed open-source energy market simulation models. The two models, namely AMIRIS and ASSUME, are both designed to simulate future energy markets using an agent-based approach. The assessment encompasses modelling features and techniques, model performance, as well as a comparison of model results, which can serve as a blueprint for future comparative studies of simulation models. The main comparison dataset includes data of Germany in 2019 and simulates the Day-Ahead market and participating actors as individual agents. Both models are comparable close to the benchmark dataset with a MAE between 5.6 and 6.4 €/MWh while also modeling the actual dispatch realistically.
Frequency mixing magnetic detection (FMMD) is a sensitive and selective technique to detect magnetic nanoparticles (MNPs) serving as probes for binding biological targets. Its principle relies on the nonlinear magnetic relaxation dynamics of a particle ensemble interacting with a dual frequency external magnetic field. In order to increase its sensitivity, lower its limit of detection and overall improve its applicability in biosensing, matching combinations of external field parameters and internal particle properties are being sought to advance FMMD. In this study, we systematically probe the aforementioned interaction with coupled Néel–Brownian dynamic relaxation simulations to examine how key MNP properties as well as applied field parameters affect the frequency mixing signal generation. It is found that the core size of MNPs dominates their nonlinear magnetic response, with the strongest contributions from the largest particles. The drive field amplitude dominates the shape of the field-dependent response, whereas effective anisotropy and hydrodynamic size of the particles only weakly influence the signal generation in FMMD. For tailoring the MNP properties and parameters of the setup towards optimal FMMD signal generation, our findings suggest choosing large particles of core sizes dc > 25 nm nm with narrow size distributions (σ < 0.1) to minimize the required drive field amplitude. This allows potential improvements of FMMD as a stand-alone application, as well as advances in magnetic particle imaging, hyperthermia and magnetic immunoassays.
K0 production in e+e− annihilations at 30 GeV center of mass energy. TASSO Collaboration
(1980)
Effective training requires high muscle forces potentially leading to training-induced injuries. Thus, continuous monitoring and controlling of the loadings applied to the musculoskeletal system along the motion trajectory is required. In this paper, a norm-optimal iterative learning control algorithm for the robot-assisted training is developed. The algorithm aims at minimizing the external knee joint moment, which is commonly used to quantify the loading of the medial compartment. To estimate the external knee joint moment, a musculoskeletal lower extremity model is implemented in OpenSim and coupled with a model of an industrial robot and a force plate mounted at its end-effector. The algorithm is tested in simulation for patients with varus, normal and valgus alignment of the knee. The results show that the algorithm is able to minimize the external knee joint moment in all three cases and converges after less than seven iterations.
Isomeric states in ¹³⁴ Ba
(1980)
Isomeric states in ¹³⁴ Ba
(1980)
Isomeric state in ¹³⁶ La
(1981)
Isomeric state in ¹³⁴ La
(1981)
Single-photon emission tomography (SPET) with the amino acid analogue l-3-[123I]iodo-α-methyl tyrosine (IMT) is helpful in the diagnosis and monitoring of cerebral gliomas. Radiolabelled amino acids seem to reflect tumour infiltration more specifically than conventional methods like magnetic resonance imaging and computed tomography. Automatic tumour delineation based on maximal tumour uptake may cause an overestimation of mean tumour uptake and an underestimation of tumour extension in tumours with circumscribed peaks. The aim of this study was to develop a program for tumour delineation and calculation of mean tumour uptake which takes into account the mean background activity and is thus optimised to the problem of tumour definition in IMT SPET. Using the frequency distribution of pixel intensities of the tomograms a program was developed which automatically detects a reference brain region and draws an isocontour region around the tumour taking into account mean brain radioactivity. Tumour area and tumour/brain ratios were calculated. A three-compartment phantom was simulated to test the program. The program was applied to IMT SPET studies of 20 patients with cerebral gliomas and was compared to the results of manual analysis by three different investigators. Activity ratios and chamber extension of the phantom were correctly calculated by the automatic analysis. A method based on image maxima alone failed to determine chamber extension correctly. Manual region of interest analysis in patient studies resulted in a mean inter-observer standard deviation of 8.7%±6.1% (range 2.7%–25.0%). The mean value of the results of the manual analysis showed a significant correlation to the results of the automatic analysis (r = 0.91, P<0.0001 for the uptake ratio; r = 0.87, P<0.0001 for the tumour area). We conclude that the algorithm proposed simplifies the calculation of uptake ratios and may be used for observer-independent evaluation of IMT SPET studies. Three-dimensional tumour recognition and transfer to co-registered morphological images based on this program may be useful for the planning of surgical and radiation treatment.
This study has been performed to design the combination of the new ClearPET (ClearPET is a trademark of the Crystal Clear Collaboration), a small animal positron emission tomography (PET) system, with a micro-computed tomography (microCT) scanner. The properties of different microCT systems have been determined by simulations based on GEANT4. We will demonstrate the influence of the detector material and the X-ray spectrum on the obtained contrast. Four different detector materials (selenium, cadmium zinc telluride, cesium iodide and gadolinium oxysulfide) and two X-ray spectra (a molybdenum and a tungsten source) have been considered. The spectra have also been modified by aluminum filters of varying thickness. The contrast between different tissue types (water, air, brain, bone and fat) has been simulated by using a suitable phantom. The results indicate the possibility to improve the image contrast in microCT by an optimized combination of the X-ray source and detector material.
This study has been performed to design the combination of the new ClearPET TM (ClearPET is a trademark of the Crystal Clear Collaboration), a small animal Positron Emission Tomography (PET) system, with a microComputed Tomography (microCT) scanner. The properties of different microCT systems have been determined by simulations based on GEANT4. We demonstrate the influence of the detector material and the X-ray spectrum on the obtained contrast. Four different detector materials (selenium, cadmium zinc telluride, cesium iodide and gadolinium oxysulfide) and two X-ray spectra (a molybdenum and a tungsten source) have been considered. The spectra have also been modified by aluminum filters of varying thickness. The contrast between different tissue types (water, air, brain, bone and fat) has been simulated by using a suitable phantom. The results indicate the possibility to improve the image contrast in microCT by an optimized combination of the X-ray source and detector material.
After a liver tumor intervention the medical doctor has to compare both pre and postoperative CT acquisitions to ensure that all carcinogenic cells are destroyed. A correct assessment of the intervention is of vital importance, since it will reduce the probability of tumor recurrence. Some methods have been proposed to support the medical doctors during the assessment process, however, all of them focus on secondary tumors. In this paper a tool is presented that enables the outcome validation for both primary and secondary tumors. Therefore, a multiphase registration (preoperative arterial and portal phases) followed by a registration between the pre and postoperative CT images is carried out. The first registration is in charge of the primary tumors that are only visible in the arterial phase. The secondary tumors will be incorporated in the second registration step. Finally, the part of the tumor that was not covered by the necrosis is quantified and visualized. The method has been tested in 9 patients, with an average registration error of 1.41 mm.