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Low-pressure mercury lamps with high-purity quartz can emit both vacuum-UV (VUV, 185 nm) and UV (254 nm) and are commercially available and promising for eliminating recalcitrant organic pollutants. The feasibility of VUV/UV as a chemical-free oxidation process was verified and quantitatively assessed by the concept of H2O2 equivalence (EQH2O2), at which UV/H2O2 showed the same performance as VUV/UV for the degradation of trace organic contaminants (TOrCs). Although VUV showed superior H2O activation and oxidation performance, its performance highly varied as a function of light path length (Lp) in water, while that of UV/H2O2 proportionally decreased with decreasing H2O2 dose regardless of Lp. On increasing Lp from 1.0 to 3.0 cm, the EQH2O2 of VUV/UV decreased from 0.81 to 0.22 mM H2O2. Chloride and nitrate hardly influenced UV/H2O2, but they dramatically inhibited VUV/UV. The competitive absorbance of VUV by chloride and nitrate was verified as the main reason. The inhibitory effect was partially compensated by â¢OH formation from the propagation reactions of chloride or nitrate VUV photolysis, which was verified by kinetic modeling in Kintecus. In water with an Lp of 2.0 cm, the EQH2O2 of VUV/UV decreased from 0.43 to 0.17 mM (60.8% decrease) on increasing the chloride concentration from 0 to 15 mM and to 0.20 mM (53.5% decrease) at 4 mM nitrate. The results of this study provide a comprehensive understanding of VUV/UV oxidation in comparison to UV/H2O2, which underscores the suitability and efficiency of chemical-free oxidation with VUV/UV.
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Peróxido de Hidrogênio , Compostos Orgânicos , Oxirredução , Raios Ultravioleta , Peróxido de Hidrogênio/química , Compostos Orgânicos/química , Fotólise , Poluentes Químicos da Água/química , Nitratos/químicaRESUMO
Molecular thin carbon nanomembranes (CNMs) synthesized by electron irradiation induced cross-linking of aromatic self-assembled monolayers (SAMs) are promising 2D materials for the next generation of filtration technologies. Their unique properties including ultimately low thickness of ≈1 nm, sub-nanometer porosity, mechanical and chemical stability are attractive for the development of innovative filters with low energy consumption, improved selectivity, and robustness. However, the permeation mechanisms through CNMs resulting in, e.g., an ≈1000 times higher fluxes of water in comparison to helium have not been yet understood. Here, a study of the permeation of He, Ne, D2 , CO2 , Ar, O2 and D2 O using mass spectrometry in the temperature range from room temperature to ≈120 °C is studied. As a model system, CNMs made from [1â³,4',1',1]-terphenyl-4-thiol SAMs are investigated. It is found out that all studied gases experience an activation energy barrier upon the permeation which scales with their kinetic diameters. Moreover, their permeation rates are dependent on the adsorption on the nanomembrane surface. These findings enable to rationalize the permeation mechanisms and establish a model, which paves the way toward the rational design not only of CNMs but also of other organic and inorganic 2D materials for energy-efficient and highly selective filtration applications.
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Aliphatic amines are abundant micropollutants in wastewater treatment plant effluents. In order to mitigate such micropollutants, ozonation is one of the most commonly employed advanced treatment processes. Current research regarding ozone efficiency is heavily focusing on reaction mechanisms of different contaminant groups, including structures with amine moieties as reactive sites. This study analyzes pH-dependent reaction kinetics and pathways of gabapentin (GBP), an aliphatic primary amine with an additional carboxylic acid group. The transformation pathway was elucidated applying a novel approach using isotopically labeled ozone (18O) and quantum chemistry calculations. While the direct reaction of GBP with ozone is highly pH-dependent and slow at pH 7 (13.7 M-1 s-1), the rate constant of the deprotonated species (1.76 × 105 M-1 s-1) is comparable to those of other amine compounds. Pathway analysis based on LC-MS/MS measurements revealed that ozonation of GBP leads to the formation of a carboxylic acid group and simultaneous nitrate formation, which was also observed in the case of the aliphatic amino acid glycine. Nitrate was formed with a yield of approximately 100%. Experiments with 18O-labeled ozone demonstrated that the intermediate aldehyde does most likely not include any oxygen originating from ozone. Furthermore, quantum chemistry calculations did not provide an explanation for the C-N scission during GBP ozonation without ozone involvement, although this reaction was slightly more favorable than for respective glycine and ethylamine reactions. Overall, this study contributes to a deeper understanding of reaction mechanisms of aliphatic primary amines during wastewater ozonation.
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Ozônio , Poluentes Químicos da Água , Purificação da Água , Aminas , Gabapentina , Nitratos , Cromatografia Líquida , Espectrometria de Massas em Tandem , Cinética , Glicina , Poluentes Químicos da Água/análiseRESUMO
We present the derivation of a new kind of loss function from the symmetry rules of synchronous and asynchronous two-dimensional correlation maps. This loss function, which takes into account correlations that are based on causal relations among the members of a series of spectra, can be employed to solve non-linear inverse problems that are plagued by systematic multiplicative errors. This possibility results from the correlation-based loss function being practically insensitive to such systematic errors, which often arise in spectroscopy because sample spectra are usually ratioed against reference spectra. Using dispersion analysis, a sophisticated method of band fitting, of the spectra of poly(methyl methacrylate) films deposited on gold, we demonstrate the applicability and validity of the new loss function. If gold is used as a substrate, experimental spectra are often unphysical, that is, they display reflectance values larger than unity. In such cases, our correlation-based loss function not only helps to achieve accurate fits but also provides corrections to obtain physically meaningful spectra, which leads to results that are superior to conventional correction methods. The validity of the results is checked and proved with help of the results of dispersion analysis of spectra of films of poly(methyl methacrylate) on calcium fluoride (CaF2) and silicon (Si), which do not suffer from the systematic errors.
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Análise EspectralRESUMO
Many applications of two-dimensional materials such as graphene require the encapsulation in bulk material. While a variety of methods exist for the structural and functional characterization of uncovered 2D materials, there is a need for methods that image encapsulated 2D materials as well as the surrounding matter. In this work, we use extreme ultraviolet coherence tomography to image graphene flakes buried beneath 200â nm of silicon. We show that we can identify mono-, bi-, and trilayers of graphene and quantify the thickness of the silicon bulk on top by measuring the depth-resolved reflectivity. Furthermore, we estimate the quality of the graphene interface by incorporating a model that includes the interface roughness. These results are verified by atomic force microscopy and prove that extreme ultraviolet coherence tomography is a suitable tool for imaging 2D materials embedded in bulk materials.
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We present a tabletop setup for extreme ultraviolet (EUV) reflection spectroscopy in the spectral range from 40 to 100 eV by using high-harmonic radiation. The simultaneous measurements of reference and sample spectra with high energy resolution provide precise and robust absolute reflectivity measurements, even when operating with spectrally fluctuating EUV sources. The stability and sensitivity of EUV reflectivity measurements are crucial factors for many applications in attosecond science, EUV spectroscopy, and nano-scale tomography. We show that the accuracy and stability of our in situ referencing scheme are almost one order of magnitude better in comparison to subsequent reference measurements. We demonstrate the performance of the setup by reflective near-edge x-ray absorption fine structure measurements of the aluminum L2/3 absorption edge in α-Al2O3 and compare the results to synchrotron measurements.
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Conventional water disinfection methods such as chlorination typically involve the generation of harmful disinfection byproducts and intensive chemical consumption. Emerging electroporation disinfection techniques using nanowire-enhanced local electric fields inactivate microbes by damaging their outer structures without byproduct formation or chemical dosing. However, this physical-based method suffers from a limited inactivation efficiency under high water flux due to an insufficient contact time. Herein, we integrate electrochlorination with nanowire-enhanced electroporation to achieve a synergistic flow-through process for efficient water disinfection targeting bacteria and viruses. Electroporation at the cathode induces sub-lethal damages on the microbial outer structures. Subsequently, electrogenerated active chlorine at the anode aggravates these electroporation-induced injuries to the level of lethal damage. This sequential flow-through disinfection system achieves complete disinfection (>6.0-log) under a very high water flux of 2.4 × 104 L/(m2 h) with an applied voltage of 2.0 V. This disinfection efficiency is 8 times faster than that of electroporation alone. Further, the specific energy consumption for the disinfection by this novel process is extremely low (8 × 10-4 kW h/m3). Our results demonstrate a promising method for rapid and energy-efficient water disinfection by coupling electroporation with electrochlorination to meet vital needs for pathogen elimination.
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Nanofios , Purificação da Água , Cloro/química , Desinfecção , Eletroporação , Nanofios/química , Água , Purificação da Água/métodosRESUMO
HINTERGRUND: Die COVID-19 Pandemie hat zu massiven gesellschaftlichen und wirtschaftlichen Einschränkungen geführt. Im Kindesalter wurden elektive Vorsorgeuntersuchung oftmals nicht wahrgenommen und es zeigte sich eine Reduktion der Zahl der Notfallvorstellungen. MATERIAL UND METHODEN: In einer retrospektiven Studie erfolgte eine quantitative Auswertung aller Notfallpatienten der 5 Kindernotaufnahmen Hamburgs und der Kinder- und Jugendarztpraxen der Jahre 2019 und 2020. Zusätzlich erfolgte die detaillierte Analyse der Notfallbehandlungen des Altonaer Kinderkrankenhauses während der ersten Phase der Pandemie im Vergleich zum Vorjahr. Zusammenhänge zu den Eckpunkten der Pandemieentwicklung wurden analysiert. Die Berechnung signifikanter Unterschiede in Bezug auf die demographischen Daten und Krankheitsbilder erfolgte mittels Chi- Quadrat und t-Test. ERGEBNISSE: In allen 5 pädiatrischen Notaufnahmen Hamburgs zeigte sich eine nahezu gleichförmige Abnahme der Patientenvorstellungen während der Pandemie, ähnlich in den Kinder- und Jugendarztpraxen. Die Zahl der Behandlungen verhielt sich dabei nicht streng gegenläufig zu den Neuinfektionen, sondern korreliert eher mit den Mobilitätsdaten und entsprach somit den gesamtgesellschaftlichen Veränderungen. Während der Pandemie stieg der Anteil häuslicher Unfälle an der Gesamtzahl der Vorstellungen signifikant an. Die Analyse der Diagnosen zeigte unter anderem eine relative Abnahme von (viralen) Infektionskrankheiten. Nicht behandlungspflichtige Erkrankungen führten in der Pandemie seltener zur Vorstellung. Diese Phänomene entlasteten einerseits die Notaufnahmen, bergen aber auch die Gefahr, dass Erkrankungen durch Eltern falsch eingeschätzt werden und eine notwendige ärztliche Vorstellung somit zu spät erfolgt.
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COVID-19 , Serviços Médicos de Emergência , Criança , Humanos , Pandemias , SARS-CoV-2RESUMO
Using two different types of impedance biochips (PS5 and BS5) with ring top electrodes, a distinct change of measured impedance has been detected after adding 1-5 µL (with dead or live Gram-positive Lysinibacillus sphaericus JG-A12 cells to 20 µL DI water inside the ring top electrode. We relate observed change of measured impedance to change of membrane potential of L. sphaericus JG-A12 cells. In contrast to impedance measurements, optical density (OD) measurements cannot be used to distinguish between dead and live cells. Dead L. sphaericus JG-A12 cells have been obtained by adding 0.02 mg/mL of the antibiotics tetracycline and 0.1 mg/mL chloramphenicol to a batch with OD0.5 and by incubation for 24 h, 30 °C, 120 rpm in the dark. For impedance measurements, we have used batches with a cell density of 25.5 × 108 cells/mL (OD8.5) and 270.0 × 108 cells/mL (OD90.0). The impedance biochip PS5 can be used to detect the more resistive and less capacitive live L. sphaericus JG-A12 cells. Also, the impedance biochip BS5 can be used to detect the less resistive and more capacitive dead L. sphaericus JG-A12 cells. An outlook on the application of the impedance biochips for high-throughput drug screening, e.g., against multi-drug-resistant Gram-positive bacteria, is given.
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Técnicas Bacteriológicas/instrumentação , Técnicas Bacteriológicas/métodos , Espectroscopia Dielétrica/métodos , Viabilidade Microbiana , Bacillaceae , Espectroscopia Dielétrica/instrumentação , Eletrodos , Dispositivos Lab-On-A-Chip , Microscopia/métodos , Microscopia de Força Atômica , SilícioRESUMO
CaF2 seems to be the ideal substrate material for the infrared spectroscopy of organic and biological layers, since its refractive index is very similar to that of these materials. As a consequence of this similarity, the baseline, i.e., the signal strength in nonabsorbing regions, is nearly flat and does not show notable interference fringes. Nevertheless, as absorption is always accompanied by changes of the refractive index, the refractive indices of substrate and layer can substantially deviate around absorption bands. As a consequence, changes in band intensity, shape, and position result, which aggravate a correct interpretation of the spectra. For layers with thicknesses between 1 and 2 µm, we show experimentally, that deviations from the Beer-Lambert law of up to ±10% occur. Calculations reveal that for thinner layers these deviations are even higher. These results suggest the application of a wave-optics based formalism to correct the deviations. We introduce such a formalism and prove that it is able to remove the errors. In addition, it also corrects band shape and position changes.
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It has been well recognized that infrared spectra of microscopically heterogeneous media do not merely reflect the absorption of the sample but are influenced also by geometric factors and the wave nature of light causing scattering, reflection, interference, etc. These phenomena often occur simultaneously in complex samples like tissues and manifest themselves as intense baseline profiles, fringes, band distortion and band intensity changes in a measured IR spectrum. The information on the molecular level contained in IR spectra is thus entangled with the geometric structure of a sample and the optical model behind it, which largely hinders the data interpretation and in many cases renders the Beer-Lambert law invalid. It is required to recover the pure absorption (i.e., absorbance) of the sample from the measurement (i.e., apparent absorbance), that is, to remove the 'artefacts' caused merely by optical influences. To do so, we propose an artefact removal approach based on a deep convolutional neural network (CNN), specifically a 1-dimensional U-shape convolutional neural network (1D U-Net), and based our study on poly(methyl methacrylate) (PMMA) as materials. To start, a simulated dataset composed of apparent absorbance and absorbance pairs was generated according to the Mie-theory for PMMA spheres. After a data augmentation procedure, this dataset was utilized to train the 1D U-Net aiming to transform the input apparent absorbance into the corrected absorbance. The performance of the artefact removal was evaluated by the hit-quality-index (HQI) between the corrected and the true absorbance. Based on the prediction and the HQI of two experimental and one simulated independent testing datasets, we could demonstrate that the network was able to retrieve the absorbance very well, even in cases where the absorbance is completely overwhelmed by extremely large 'artefacts'. As the testing datasets bear different patterns of absorbance and 'artefacts' to the training data, the promising correction also indicated a good generalization performance of the 1D U-Net. Finally, the reliability and computational mechanism of the trained network were illustrated via two interpretation approaches including a direct visualization of layer-wise outputs as well as a saliency-based method.
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Substantial refractive index mismatches between substrate and layers lead to undulating baselines, which are known as interference fringes. These fringes can be attributed to multiple reflections inside the layers. For thin and plane parallel layers, these multiple reflections result in wave interference and electric field intensities which strongly depend on the location within the layer and wavenumber. In particular, the average electric field intensity is increased in spectral regions where the reflectance is reduced. Therefore, the most important precondition for the Beer-Lambert law to hold, absorption as the single reason for electric field intensity changes, is no longer valid and, since absorption is proportional to the electric field intensity, considerable deviations from the Beer-Lambert law result. Fringe removal is consequently synonymous with correcting deviations from the Beer-Lambert law in the spectra. Within this contribution, we introduce an appropriate formalism based on wave optics, which allows a particularly fast and simple correction of any interference based effects. We applied our approach for correcting transmittance spectra of Poly(methyl methacrylate) layers on silicon substrates. The interference effects were successfully removed and correct baselines, in good agreement with the calculated spectra, were obtained. Due to its sound theoretical foundation, our formalism can be used as benchmark to test the performance of other methods for interference fringe removal.
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Understanding the impact of geometric changes on the properties of otherwise symmetric nanostructures is of essential importance for nanophotonics. In this Letter, we show that intra- and inter-unit cell symmetry breaking can substantially modify the optical properties of nanotrimers from both the experimental and simulation aspect. Specifically, shifting the location of one nano-dot within the trimer unit cell leads to the formation of magnetic Fano resonances with loop-like polarization patterns that are not present in the symmetric configuration. We further unlock the impact of lattice modification on the optical response of square arrays of trimers with broken three-fold rotation symmetry and with intra-trimer distances as small as 25 nm, showing distinctively different spectral evolutions of the electric and magnetic Fano resonances. The results achieved highlight the symmetry breaking as an essential tool to unlock and strengthen predefined resonances, which can have important applications, particularly in the field of sensing.
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The discharge of wastewater effluents to a stream that is subsequently used for drinking water abstraction has been previously referred to as de facto water reuse. Where the abstraction of surface water for drinking water production occurs via induced bank filtration or aquifer recharge, additional site-specific factors should be considered to assess the impact of wastewater effluents on bank-filtered water. This study represents the first national reconnaissance to quantify wastewater effluent contributions in streams across Germany and consequences for indirect drinking water abstraction from these streams. An automated assessment using ArcGIS was conducted for river basins considering minimum and mean average discharge conditions of streams as well as discharge from more than 7500 wastewater facilities. In urban areas, where the natural base discharge is low, wastewater effluent contributions greater than 30-50% were determined under mean minimum discharge conditions, which commonly prevail from May to September. A conceptual model was proposed to estimate critical bank filtrate shares resulting in exceedances of monitoring trigger levels for health-relevant chemicals as a universal qualitative assessment regarding the relevance of de facto reuse conditions in surface waters used for drinking water abstraction. This approach was validated using chemical monitoring data for three case study locations.
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Água Potável , Poluentes Químicos da Água , Alemanha , Rios , Águas Residuárias , Abastecimento de ÁguaRESUMO
Raman spectroscopy in combination with appropriate sample preparation strategies, for example, enrichment of bacteria on metal surfaces, has been proven to be a promising approach for rapidly diagnosing infectious diseases. Unfortunately, the fabrication of the required chip substrates is usually very challenging due to the lack of feasible instruments that can be used for quality control in the surface modification process. The intrinsically weak Raman signal of the biomolecules, employed for the enrichment of the micro-organisms on the chip surface, does not allow for monitoring of the successful immobilization by means of a Raman spectroscopic approach. Within this contribution, we demonstrate how a simple modification of a plain aluminum surface enables enhancement (or a decrease, if desired) of the Raman signal of molecules deposited on that surface. The manipulation of the Raman signal strength is achieved via exploiting interference effects that occur, if the highly reflective aluminum surface is modified with thin layers of transparent dielectrics like aluminum oxide. The thicknesses of these layers were determined by theoretical considerations and calculations. For the first time, it is shown that the interference effects can be used for the detection of biomolecules as well by investigating the siderophore ferrioxamine B. The observed degree of enhancement was approximately 1 order of magnitude. Moreover, the employed aluminum/aluminum oxide layers have been thoroughly characterized using atomic force and scanning electron microscopy as well as X-ray reflectometry and UV-Vis measurements.
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Óxido de Alumínio/química , Alumínio/química , Desferroxamina/química , Compostos Férricos/química , Polimetil Metacrilato/química , Análise Espectral Raman/instrumentação , Desenho de Equipamento , Propriedades de SuperfícieRESUMO
A hybrid formalism combining elements from Kramers-Kronig based analyses and dispersion analysis was developed, which allows removing interference-based effects in the infrared spectra of layers on highly reflecting substrates. In order to enable a highly convenient application, the correction procedure is fully automatized and usually requires less than a minute with non-optimized software on a typical office PC. The formalism was tested with both synthetic and experimental spectra of poly(methyl methacrylate) on gold. The results confirmed the usefulness of the formalism: apparent peak ratios as well as the interference fringes in the original spectra were successfully corrected. Accordingly, the introduced formalism makes it possible to use inexpensive and robust highly reflecting substrates for routine infrared spectroscopic investigations of layers or films the thickness of which is limited by the imperative that reflectance absorbance must be smaller than about 1. For thicker films the formalism is still useful, but requires estimates for the optical constants.
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It is widely assumed that biodegradation of trace organic chemicals (TOrCs) in managed aquifer recharge (MAR) systems occurs via a cometabolic transformation with dissolved organic carbon serving as primary substrate. Hence, the composition facilitating bioavailability of the organic matter seems to have a great impact on TOrCs transformation in MAR systems. The aim of this study was to elucidate the character of effluent organic matter present in the feedwater of a simulated sequential MAR system throughout the infiltration by use of FT-ICR-MS analyses as well as spectroscopic methods. Furthermore, compositional changes were correlated with TOrCs targeted throughout the system as well as the abundance of different microbial phyla. On the basis of their behavior throughout the infiltration system in which different redox and substrate conditions prevailed, TOrCs were classified in four groups: easily degradable, redox insensitive, redox sensitive, and persistent. Masses correlating with persistent TOrCs were mainly comprised of CHNO-containing molecules but also of CHO which are known as carboxyl-rich alicyclic molecules, while CHOS and CHNOS can be neglected. Easily degradable TOrCs could be associated with CHNO-, CHO-, and CHOS-containing compounds. However, a shift of molecular compounds to mostly CHOS was observed for redox-insensitive TOrCs. Three hundred thirty eight masses correlated with removal of redox-sensitive TOrCs, but no distinct clustering was identified.
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Água Subterrânea , Microbiota , Poluentes Químicos da Água , Purificação da Água , Biodegradação Ambiental , Compostos OrgânicosRESUMO
Surface-enhanced Raman spectroscopy (SERS) enables sensitive chemical studies and materials identification, relying on electromagnetic (EM) and chemical-enhancement mechanisms. Here we introduce a tool for the correlative nanoimaging of EM and SERS hotspots, areas of strongly enhanced EM fields and Raman scattering, respectively. To that end, we implemented a grating spectrometer into a scattering-type scanning near-field optical microscope (s-SNOM) for mapping of both the elastically and inelastically (Raman) scattered light from the near-field probe, that is, a sharp silicon tip. With plasmon-resonant gold dimers (canonical SERS substrates) we demonstrate with nanoscale spatial resolution that the enhanced Raman scattering from the tip is strongly correlated with its enhanced elastic scattering, the latter providing access to the EM-field enhancement at the illumination frequency. Our technique has wide application potential in the correlative nanoimaging of local-field enhancement and SERS efficiency as well as in the investigation and quality control of novel SERS substrates.
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We isolated the plasmonic contribution to surface-enhanced Raman scattering (SERS) and found it to be much stronger than expected. Organic dyes encapsulated in single-walled carbon nanotubes are ideal probes for quantifying plasmonic enhancement in a Raman experiment. The molecules are chemically protected through the nanotube wall and spatially isolated from the metal, which prevents enhancement by chemical means and through surface roughness. The tubes carry molecules into SERS hotspots, thereby defining molecular position and making it accessible for structural characterization with atomic-force and electron microscopy. We measured a SERS enhancement factor of 106 on α-sexithiophene (6T) molecules in the gap of a plasmonic nanodimer. This is two orders of magnitude stronger than predicted by the electromagnetic enhancement theory (104). We discuss various phenomena that may explain the discrepancy (including hybridization, static and dynamic charge transfer, surface roughness, uncertainties in molecular position and orientation), but found all of them lacking in enhancement for our probe system. We suggest that plasmonic enhancement in SERS is, in fact, much stronger than currently anticipated. We discuss novel approaches for treating SERS quantum mechanically that appear promising for predicting correct enhancement factors. Our findings have important consequences on the understanding of SERS as well as for designing and optimizing plasmonic substrates.
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Plasmon-based sensors are excellent tools for a label-free detection of small biomolecules. An interesting group of such sensors are plasmonic nanorulers that rely on the plasmon hybridization upon modification of their morphology to sense nanoscale distances. Sensor geometries based on the interaction of plasmons in a flat metallic layer together with metal nanoparticles inherit unique advantages but need a special optical excitation configuration that is not easy to miniaturize. Herein, we introduce the concept of nanoruler excitation by direct, electrically induced generation of surface plasmons based on the quantum shot noise of tunneling currents. An electron tunneling junction consisting of a metal-dielectric-semiconductor heterostructure is directly incorporated into the nanoruler basic geometry. With the application of voltage on this modified nanoruler, the plasmon modes are directly excited without any additional optical component as a light source. We demonstrate via several experiments that this electrically driven nanoruler possesses similar properties as an optically exited one and confirm its sensing capabilities by the detection of the binding of small biomolecules such as antibodies. This new sensing principle could open the way to a new platform of highly miniaturized, integrated plasmonic sensors compatible with monolithic integrated circuits.