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Abstract Ultra-intense lasers that ionize atoms and accelerate electrons in solids to near the speed of light can lead to kinetic instabilities that alter the laser absorption and subsequent electron transport, isochoric heating, and ion acceleration. These instabilities can be difficult to characterize, but X-ray scattering at keV photon energies allows for their visualization with femtosecond temporal resolution on the few nanometer mesoscale. Here, we perform such experiment on laser-driven flat silicon membranes that shows the development of structure with a dominant scale of 60 nm in the plane of the laser axis and laser polarization, and 95 nm in the vertical direction with a growth rate faster than 0.1 fs−1. Combining the XFEL experiments with simulations provides a complete picture of the structural evolution of ultra-fast laser-induced plasma density development, indicating the excitation of plasmons and a filamentation instability. Particle-in-cell simulations confirm that these signals are due to an oblique two-stream filamentation instability. These findings provide new insight into ultra-fast instability and heating processes in solids under extreme conditions at the nanometer level with possible implications for laser particle acceleration, inertial confinement fusion, and laboratory astrophysics.

Advanced oxidation processes (AOPs) are a growing research field with a large variety of different process variants and materials being tested at laboratory scale. However, despite extensive research in recent years and decades, many variants have not been transitioned to pilot- and full-scale operation. One major concern are the inconsistent experimental approaches applied across different studies that impede identification, comparison, and upscaling of the most promising AOPs. The aim of this tutorial review is to streamline future studies on the development of new solutions and materials for advanced oxidation by providing guidance for comparable and scalable oxidation experiments. We discuss recent developments in catalytic, ozone-based, radiation-driven, and other AOPs, and outline future perspectives and research needs. Since standardized experimental procedures are not available for most AOPs, we propose basic rules and key parameters for lab-scale evaluation of new AOPs including selection of suitable probe compounds and scavengers for the measurement of (major) reactive species. A two-phase approach to assess new AOP concepts is proposed, consisting of (i) basic research and proof-of-concept (technology readiness levels (TRL) 1–3), followed by (ii) process development in the intended water matrix including a cost comparison with an established process, applying comparable and scalable parameters such as UV fluence or ozone consumption (TRL 3–5). Subsequent demonstration of the new process (TRL 6–7) is briefly discussed, too. Finally, we highlight important research tools for a thorough mechanistic process evaluation and risk assessment including screening for transformation products that should be based on chemical logic and combined with complementary tools (mass balance, chemical calculations).

Biosensors are used for the specific and sensitive detection of biomolecules. In conventional approaches, the suspected target molecules are bound to selected capture molecules and successful binding is indicated by additional labelling to enable optical readout. This labelling requires additional processing steps tailored to the application. While numerous label-free interaction assays exist, they often compromise on detection characteristics. In this context, we introduce a novel diffractometric biosensor, comprising a diffractive biosensor chip and an associated optical reader assembly. This innovative system can capture an entire assay, detecting various types of molecules in a label-free manner and present the results within in a single, comprehensive image. The applicability of the biosensor is assessed for the detection of viral DNA as well as proteins directly in human plasma, investigating different antigens. In our experiments, we achieve a detection limit of 4.2 pg/mm², which is comparable to other label-free optical biosensors. The simplicity and robustness of the method make it a compelling option for advancing biosensing technologies. This work contributes to the development of an imaging diffractometric biosensor with the potential for multiple applications in molecular interaction analysis.

Memristors, since their inception, have demonstrated remarkable characteristics, notably the exceptional reconfigurability of their memory. This study delves into electroforming-free YMnO3 (YMO)-based resistive switches, emphasizing the reconfigurable memory effect in multiferroic YMO thin films with metallically conducting electrodes and their pivotal role in achieving adaptable frequency responses in impedance circuits consisting of reconfigurable YMO-based resistive switches and no reconfigurable passive elements, e.g., inductors and capacitors. The multiferroic YMO possesses a network of charged domain walls which can be reconfigured by a time-dependent voltage applied between the metallically conducting electrodes. Through experimental demonstrations, this study scrutinizes the impedance response not only for individual switch devices but also for impedance circuitry based on YMO resistive switches in both low- and high-resistance states, interfacing with capacitors and inductors in parallel and series configurations. Scrutinized Nyquist plots visually capture the intricate dynamics of impedance circuitry, revealing the potential of electroforming-free YMO resistive switches in finely tuning frequency responses within impedance circuits. This adaptability, rooted in the unique properties of YMO, signifies a paradigm shift heralding the advent of advanced and flexible electronic technologies.

We introduce OrbiFragsNets, a tool for automatic annotation of MS2 spectra generated by Orbitrap instruments, as well as the concepts of chemical consistency and fragments networks. OrbiFragsNets takes advantage of the specific confidence interval for each peak in every MS2 spectrum, which is an unclear idea across the high-resolution mass spectrometry literature. The spectrum annotations are expressed as fragments networks, a set of networks with the possible combinations of annotations for the fragments. The model behind OrbiFragsNets is briefly described here and explained in detail in the constantly updated manual available in the GitHub repository. This new approach in MS2 spectrum de novo automatic annotation proved to perform as good as well established tools such as RMassBank and SIRIUS. • A new approach on automatic annotation of Orbitrap MS2 spectra is introduced. • Possible spectrum annotation are described as independent consistent networks, with annotations for each fragment as nodes, and annotations for the mass difference between fragments as edges. • Annotation process is described as the selection of the most connected fragments network.

Abstract Organic semiconductors (OSC) are widely used for consumer electronic products owing to their attractive properties such as flexibility and low production cost. Atomically thin transition metal dichalcogenides (TMDs) are another class of emerging materials with superior electronic and optical properties. Integrating them into van der Waals (vdW) heterostructures provides an opportunity to harness the advantages of both material systems. However, building such heterojunctions by conventional physical vapor deposition (PVD) of OSCs is challenging, since the growth is disrupted due to limited diffusion of the molecules on the TMD surface. Here we report wafer-scale (3-inch) fabrication of transferable OSC nanosheets with thickness down to 15 nm, which enable the realization of heterojunction devices. By controlled dissolution of a poly(acrylic acid) film, on which the OSC films were grown by PVD, they can be released and transferred onto arbitrary substrates. OSC crystal quality and optical anisotropy are preserved during the transfer process. By transferring OSC nanosheets (p-type) onto prefabricated electrodes and TMD monolayers (n-type), we fabricate and characterize various electronic devices including unipolar, ambipolar and antiambipolar field-effect transistors. Such vdW p-n heterojunction devices open up a wide range of possible applications ranging from ultrafast photodetectors to conformal electronics.

Supercritical angle localisation microscopy (SALM) allows the z-positions of single fluorophores to be extracted from the intensity of supercritical angle fluorescence. Here the authors improve the z-resolution of SALM, and report nanometre isotropic localisation precision on DNA origami structures.

Tertiary wastewater treatment could provide a reliable source of water for reuse. Amongst these types of wastewater treatment, deep-bed filtration of secondary effluents can effectively remove particles and organic matter; however, NH4+ and NO2− are not easily removed. This study examined the feasibility of stimulating microbial activity using hydrogen peroxide (H2O2) as a bio-specific and clean oxygen source that leaves no residuals in the water and is advantageous upon aeration due to the solubility limitations of the oxygen. The performance of a pilot bio-filtration system at a filtration velocity of 5−6 m/h, was enhanced by the addition of H2O2 for particle, organic matter, NH4+, and NO2− removal. Hydrogen peroxide provided the oxygen demand for full nitrification. As a result, influent concentrations of 4.2 ± 2.5 mg/L N-NH4+ and 0.65 ± 0.4 mg/L N-NO2 were removed during the short hydraulic residence time (HRT). In comparison, filtration without H2O2 addition only removed up to 0.6 mg/L N-NH4+ and almost no N-NO2−. A DNA metagenome analysis of the functional genes of the media biomass reflected a significant potential for simultaneous nitrification and denitrification activity. It is hypothesized that the low biodegradability of the organic carbon and H2O2 addition stimulated oxygen utilization in favor of nitrification, followed by the enhancement of anoxic activity.

The focusing of light represents a key functionality, which can efficiently be achieved through wavefront shaping via metasurfaces (MSs). Remote light focusing requires interfacing these ultraflat photonic structures with optical fibers, which is hard to achieve due to fabrication limitations and challenging beam management. Herein, the successful interfacing of a focusing plasmonic metalens with a regular single‐mode step‐index fiber through modified electron beam lithography is demonstrated. Specifically, a plasmonic MS consisting of nanoslots is realized on the end face of a modified single‐mode fiber via planarization and e‐beam lithography. A key feature of the device is the introduction of a coreless glass section in between the fiber and MS, which allows for free beam expansion up to 48 μm to fully exploit the numerical aperture (NA) of the metalens. In agreement with simulations, a clear focus with a NA of about 0.3 is found in the experiments, confirming the successful realization of a plasmonic metalens‐enhanced single‐mode fiber. Due to its unique properties, this concept finds applications in a multitude of areas, examples of which include optical trapping, generation of sophisticated beam profiles, and boosting light coupling efficiencies.

Extreme states of matter exist throughout the universe, e.g., inside planetary cores, stars, or astrophysical jets. Such conditions can be generated in the laboratory in the interaction of powerful lasers with solids. Yet, the measurement of the subsequent plasma dynamics with regard to density, temperature, and ionization is a major experimental challenge. However, ultrashort x-ray pulses provided by x-ray free electron lasers (XFELs) allow for dedicated studies, which are highly relevant to study laboratory astrophysics, laser-fusion research, or laser-plasma-based particle acceleration. Here we report on experiments that employ a novel ultrafast method, which allows us to simultaneously access temperature, ionization state, and nanometer scale expansion dynamics in high-intensity, laser-driven, solid-density plasmas with a single x-ray detector. Using this method, we gain access to the expansion dynamics of a buried layer in compound samples, and we measure opacity changes arising from bound-bound resonance transitions in highly ionized copper. The presence of highly ionized copper leads to a temperature estimate of at least 2 million Kelvin already after the first 100 fs following the high-intensity laser irradiation. More specifically, we make use of asymmetries in small-angle x-ray scattering (SAXS) patterns, which arise from different spatial distributions of absorption and scattering cross sections in nanostructured grating samples when we tune an XFEL to atomic resonant energies of copper. Thereby, changes in asymmetry can be connected with the evolution of the plasma expansion and ionization dynamics. The potential of XFEL-based resonant SAXS to obtain three-dimensional ultrafast, nanoscopic information on density and opacity may offer a unique path for the characterization of dynamic processes in high energy density plasmas.

The efficient incoupling of light into particular fibers at large angles is essential for a multitude of applications; however, this is difficult to achieve with commonly used fibers due to low numerical aperture. Here, we demonstrate that commonly used optical fibers functionalized with arrays of metallic nanodots show substantially improved large-angle light-collection performances at multiple wavelengths. In particular, we show that at visible wavelengths, higher diffraction orders contribute significantly to the light-coupling efficiency, independent of the incident polarization, with a dominant excitation of the fundamental mode. The experimental observation is confirmed by an analytical model, which directly suggests further improvement in incoupling efficiency through the use of powerful nanostructures such as metasurface or dielectric gratings. Therefore, our concept paves the way for high-performance fiber-based optical devices and is particularly relevant within the context of endoscopic-type applications in life science and light collection within quantum technology.

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.

In 2015, the town of El Port de la Selva in Spain implemented soil-aquifer treatment (SAT) using tertiary treated wastewater effluents to replenish the local potable aquifer. This study evaluated the initial phase of this indirect potable water reuse system including a characterization of hydraulic conditions in the aquifer and monitoring of microbial contaminants and 151 chemicals of emerging concern (CECs). The combined treatment resulted in very low abundances of indicator bacteria, enteric viruses and phages in the monitoring wells after three days of infiltration and a reduction of antibiotic microbial resistance to background levels of local groundwater. After tertiary treatment, 94 CECs were detected in the infiltration basin of which 15 chemicals exceeded drinking water thresholds or health-based monitoring trigger levels. Although SAT provided an effective barrier for many chemicals, 5 CECs were detected above health-based threshold levels in monitoring wells after short hydraulic retention times. However, additional attenuation is expected due to dilution prior to abstraction via downstream drinking water wells and during granular activated carbon (GAC) filtration, which was recently installed to mitigate residual CECs. Overall, the results demonstrate that indirect potable water reuse can be a reliable option for smaller communities, if related risks from microbial and chemical contaminants are adequately addressed by tertiary treatment and subsequent SAT, providing sufficient hydraulic retention times for pathogen decay and CEC removal.

We counted bacterial cells of E. coli strain K12 in several-microliter DI water or in several-microliter PBS in the low optical density (OD) range (OD = 0.05–1.08) in contact with the surface of Si-based impedance biochips with ring electrodes by impedance measurements. The multiparameter fit of the impedance data allowed calibration of the impedance data with the concentration cb of the E. coli cells in the range of cb = 0.06 to 1.26 × 109 cells/mL. The results showed that for E. coli in DI water and in PBS, the modelled impedance parameters depend linearly on the concentration of cells in the range of cb = 0.06 to 1.26 × 109 cells/mL, whereas the OD, which was independently measured with a spectrophotometer, was only linearly dependent on the concentration of the E. coli cells in the range of cb = 0.06 to 0.50 × 109 cells/mL.

Deionized water and glucose without yeast and with yeast (Saccharomyces cerevisiae) of optical density OD600 that ranges from 4 to 16 has been put in the ring electrode region of six different types of impedance biochips and impedance has been measured in dependence on the added volume (20, 21, 22, 23, 24, 25 µL). The measured impedance of two out of the six types of biochips is strongly sensitive to the addition of both liquid without yeast and liquid with yeast and modelled impedance reveals a linear relationship between the impedance model parameters and yeast concentration. The presented biochips allow for continuous impedance measurements without interrupting the cultivation of the yeast. A multiparameter fit of the impedance model parameters allows for determining the concentration of yeast (cy) in the range from cy = 3.3 × 107 to cy = 17 × 107 cells/mL. This work shows that independent on the liquid, i.e., DI water or glucose, the impedance model parameters of the two most sensitive types of biochips with liquid without yeast and with liquid with yeast are clearly distinguishable for the two most sensitive types of biochips.

In this work, we report on the impedance of p-n junction-based Si biochips with gold ring top electrodes and unstructured platinum bottom electrodes which allows for counting target biomaterial in a liquid-filled ring top electrode region. The systematic experiments on p-n junction-based Si biochips fabricated by two different sets of implantation parameters (i.e. biochips PS5 and BS5) are studied, and the comparable significant change of impedance characteristics in the biochips in dependence on the number of bacteria suspension, i.e., Lysinibacillus sphaericus JG-A12, in Deionized water with an optical density at 600 nm from OD600 = 4–16 in the electrode ring region is demonstrated. Furthermore, with the help of the newly developed two-phase electrode structure, the modeled capacitance and resistance parameters of the electrical equivalent circuit describing the p-n junction-based biochips depend linearly on the number of bacteria in the ring top electrode region, which successfully proves the potential performance of p-n junction-based Si biochips in observing the bacterial suspension. The proposed p-n junction-based biochips reveal perspective applications in medicine and biology for diagnosis, monitoring, management, and treatment of diseases.

In order to combine the advantages of fluorescence and surface-enhanced Raman spectroscopy (SERS) on the same chip platform, a nanostructured gold surface with a unique design, allowing both the sensitive detection of fluorescence light together with the specific Raman fingerprint of the fluorescent molecules, was established. This task requires the fabrication of plasmonic arrays that permit the binding of molecules of interest at different distances from the metallic surface. The most efficient SERS enhancement is achieved for molecules directly adsorbed on the metallic surface due to the strong field enhancement, but where, however, the fluorescence is quenched most efficiently. Furthermore, the fluorescence can be enhanced efficiently by careful adjustment of the optical behavior of the plasmonic arrays. In this article, the simultaneous application of SERS and fluorescence, through the use of various gold nanostructured arrays, is demonstrated by the realization of a DNA detection scheme. The results shown open the way to more flexible use of plasmonic arrays in bioanalytics.

The complex physics of the interaction between short-pulse ultrahigh-intensity lasers and solids is so far difficult to access experimentally, and the development of compact laser-based next-generation secondary radiation sources, e.g., for tumor therapy, laboratory astrophysics, and fusion, is hindered by the lack of diagnostic capabilities to probe the complex electron dynamics and competing instabilities. At present, the fundamental plasma dynamics that occur at the nanometer and femtosecond scales during the laser-solid interaction can only be elucidated by simulations. Here we show experimentally that small-angle x-ray scattering of femtosecond x-ray free-electron laser pulses facilitates new capabilities for direct in situ characterization of intense short-pulse laser-plasma interactions at solid density that allows simultaneous nanometer spatial and femtosecond temporal resolution, directly verifying numerical simulations of the electron density dynamics during the short-pulse high-intensity laser irradiation of a solid density target. For laser-driven grating targets, we measure the solid density plasma expansion and observe the generation of a transient grating structure in front of the preinscribed grating, due to plasma expansion. The density maxima are interleaved, forming a double frequency grating in x-ray free-electron laser projection for a short time, which is a hitherto unknown effect. We expect that our results will pave the way for novel time-resolved studies, guiding the development of future laser-driven particle and photon sources from solid targets.

Managed aquifer recharge (MAR) systems are an efficient barrier for many contaminants. The biotransformation of trace organic chemicals (TOrCs) strongly depends on the redox conditions as well as on the dissolved organic carbon availability. Oxic and oligotrophic conditions are favored for enhanced TOrCs removal which is obtained by combining two filtration systems with an intermediate aeration step. In this study, four parallel laboratory-scale soil column experiments using different intermittent aeration techniques were selected to further optimize TOrCs transformation during MAR: no aeration, aeration with air, pure oxygen and ozone. Rapid oxygen consumption, nitrate reduction and dissolution of manganese confirmed anoxic conditions within the first filtration step, mimicking traditional bank filtration. Aeration with air led to suboxic conditions, whereas oxidation by pure oxygen and ozone led to fully oxic conditions throughout the second system. The sequential system resulted in an equal or better transformation of most TOrCs compared to the single step bank filtration system. Despite the fast oxygen consumption, acesulfame, iopromide, iomeprol and valsartan were degraded within the first infiltration step. The compounds benzotriazole, diclofenac, 4-Formylaminoantipyrine, gabapentin, metoprolol, valsartan acid and venlafaxine revealed a significantly enhanced removal in the systems with intermittent oxidation compared to the conventional treatment without aeration. Further improvement of benzotriazole and gabapentin removal by using pure oxygen confirmed potential oxygen limitation in the second column after aeration with air. Ozonation resulted in an enhanced removal of persistent compounds (i.e., carbamazepine, candesartan, olmesartan) and further increased the attenuation of gabapentin, methylbenzotriazole, benzotriazole, and venlafaxine. Diatrizoic acid revealed little degradation in an ozone–MAR hybrid system.