Double layer acceleration of ions with differently charged states in a laser induced plasma.

The electric field driven acceleration of plasma ions is an intrinsic effect in laser-induced plasma plumes and is responsible for the generation of high-energy ions. At high laser fluences (≥ 2 J/cm2), multiply charged ions are formed and affect the plume expansion dynamics. In this paper, we used kinetic energy-resolved mass spectrometry to investigate the relative abundance and kinetic energy distributions of singly- and doubly-charged ions produced by KrF-laser ablation of nine different oxide targets. The doubly charged metal ions with a lower mass-to-charge (m/z) ratio show narrow energy distributions at high average kinetic energies coinciding with the cutoff energies for the singly-charged ion distributions. The observation suggests that the recombination of higher charged ions plays a prominent role in the formation of the high-energy tail for singly-charged ions. The results are discussed in terms of component volatility and a dynamic double layer, where ions with different m/z values experience different accelerations.

A practical guide to pulsed laser deposition.

Nanoscale thin films are widely implemented across a plethora of technological and scientific areas, and form the basis for many advancements that have driven human progress, owing to the high degree of functional tunability based on the chemical composition. Pulsed laser deposition is one of the multiple physical vapour deposition routes to fabricate thin films, employing laser energy to eject material from a target in the form of a plasma. A substrate, commonly a single-crystal oxide, is placed in the path of the plume and acts as a template for the arriving species from the target to coalesce and self-assemble into a thin film. This technique is tremendously useful to produce crystalline films, due to the wide range of atmospheric conditions and the extent of possible chemical complexity of the target. However, this flexibility results in a high degree of complexity, oftentimes requiring rigorous optimisation of the growth parameters to achieve high quality crystalline films with desired composition. In this tutorial review, we aim to reduce the complexity and the barrier to entry for the controlled growth of complex oxides by pulsed laser deposition. We present an overview of the fundamental and practical aspects of pulsed laser deposition, discuss the consequences of tailoring the growth parameters on the thin film properties, and describe in situ monitoring techniques that are useful in gaining a deeper understanding of the properties of the resultant films. Particular emphasis is placed on the general relationships between the growth parameters and the consequent structural, chemical and functional properties of the thin films. In the final section, we discuss the open questions within the field and possible directions to further expand the utility of pulsed laser deposition.

PLD plasma plume analysis: a summary of the PSI contribution.

We report on the properties of laser-induced plasma plumes generated by ns pulsed excimer lasers as used for pulsed laser deposition to prepare thin oxide films. A focus is on the time and spatial evolution of chemical species in the plasma plume as well as the mechanisms related to the plume expansion. The overall dynamics of such a plume is governed by the species composition in particular if three or more elements are involved. We studied the temporal evolution of the plume, the composition of the chemical species in the plasma, as well as their electric charge. In particular, ionized species can have an important influence on film growth. Likewise, the different oxygen sources contributing to the overall oxygen content of an oxide film are presented and discussed. Important for the growth of oxide thin films is the compositional transfer of light element such as oxygen or Li. We will show and discuss how to monitor these light elements using plasma spectroscopy and plasma imaging and outline some consequences of our experimental results. Supplementary Information: The online version contains supplementary material available at 10.1007/s00339-023-06408-4.

High-Sensitivity Ammonia Sensors with Carbon Nanowall Active Material via Laser-Induced Transfer.

Ammonia sensors with high sensitivity, reproducible response, and low cost are of paramount importance for medicine, i.e., being a biomarker to diagnose lung and renal conditions, and agriculture, given that fertilizer application and livestock manure account for more than 80% of NH3 emissions. Thus, in this work, we report the fabrication of ultra-sensitive ammonia sensors by a rapid, efficient, and solvent-free laser-based procedure, i.e., laser-induced forward transfer (LIFT). LIFT has been used to transfer carbon nanowalls (CNWs) onto flexible polyimide substrates pre-patterned with metallic electrodes. The feasibility of LIFT is validated by the excellent performance of the laser-printed CNW-based sensors in detecting different concentrations of NH3 in the air, at room temperature. The sensors prepared by LIFT show reversible responses to ammonia when exposed to 20 ppm, whilst at higher NH3 concentrations, the responses are quasi-dosimetric. Furthermore, the laser-printed CNW-based sensors have a detection limit as low as 89 ppb and a response time below 10 min for a 20 ppm exposure. In addition, the laser-printed CNW-based sensors are very robust and can withstand more than 200 bending cycles without loss of performance. This work paves the way for the application and integration of laser-based techniques in device fabrication, overcoming the challenges associated with solvent-assisted chemical functionalization.

New Insight into the Gas Phase Reaction Dynamics in Pulsed Laser Deposition of Multi-Elemental Oxides.

The gas-phase reaction dynamics and kinetics in a laser induced plasma are very much dependent on the interactions of the evaporated target material and the background gas. For metal (M) and metal-oxygen (MO) species ablated in an Ar and O2 background, the expansion dynamics in O2 are similar to the expansion dynamics in Ar for M+ ions with an MO+ dissociation energy smaller than O2. This is different for metal ions with an MO+ dissociation energy larger than for O2. This study shows that the plume expansion in O2 differentiates itself from the expansion in Ar due to the formation of MO+ species. It also shows that at a high oxygen background pressure, the preferred kinetic energy range to form MO species as a result of chemical reactions in an expanding plasma, is up to 5 eV.

Reconfigurable halide perovskite nanocrystal memristors for neuromorphic computing.

Many in-memory computing frameworks demand electronic devices with specific switching characteristics to achieve the desired level of computational complexity. Existing memristive devices cannot be reconfigured to meet the diverse volatile and non-volatile switching requirements, and hence rely on tailored material designs specific to the targeted application, limiting their universality. "Reconfigurable memristors" that combine both ionic diffusive and drift mechanisms could address these limitations, but they remain elusive. Here we present a reconfigurable halide perovskite nanocrystal memristor that achieves on-demand switching between diffusive/volatile and drift/non-volatile modes by controllable electrochemical reactions. Judicious selection of the perovskite nanocrystals and organic capping ligands enable state-of-the-art endurance performances in both modes - volatile (2 × 106 cycles) and non-volatile (5.6 × 103 cycles). We demonstrate the relevance of such proof-of-concept perovskite devices on a benchmark reservoir network with volatile recurrent and non-volatile readout layers based on 19,900 measurements across 25 dynamically-configured devices.

Linking Brain Structure, Activity, and Cognitive Function through Computation.

Understanding the human brain is a "Grand Challenge" for 21st century research. Computational approaches enable large and complex datasets to be addressed efficiently, supported by artificial neural networks, modeling and simulation. Dynamic generative multiscale models, which enable the investigation of causation across scales and are guided by principles and theories of brain function, are instrumental for linking brain structure and function. An example of a resource enabling such an integrated approach to neuroscientific discovery is the BigBrain, which spatially anchors tissue models and data across different scales and ensures that multiscale models are supported by the data, making the bridge to both basic neuroscience and medicine. Research at the intersection of neuroscience, computing and robotics has the potential to advance neuro-inspired technologies by taking advantage of a growing body of insights into perception, plasticity and learning. To render data, tools and methods, theories, basic principles and concepts interoperable, the Human Brain Project (HBP) has launched EBRAINS, a digital neuroscience research infrastructure, which brings together a transdisciplinary community of researchers united by the quest to understand the brain, with fascinating insights and perspectives for societal benefits.

Stimulating effect of hydrostatic pressure on ultrasonic sewage sludge treatment for COD solubilization and methane production.

The performance of ultrasonic treatment was assessed under different hydrostatic pressures for two different waste activated sludges. The impact of pressurized sonication was evaluated based on the degree of disintegration (DDCOD) and the specific methane yield (SMY). An enhancement of DDCOD was observed at an intermediate pressure level (max. 53% at 1.0 bar), but at higher pressure levels (up to 3.5 bar), the enhancement was not as pronounced as for the intermediate ranges (max. 11%). In contrast to DDCOD, SMY increased with increasing pressure for both sludge samples tested (max 17% at 3.5 bar) so that SMY did not show a notable correlation with DDCOD. A positive energy balance (max. 167%) considering the energy input for ultrasonication and the additional methane generated was only achieved in samples treated under elevated hydrostatic pressure. Since this can be achieved with negligible effort, the enhancement can be considered as "methane for free".

Lessons learned from urgent computing in Europe: Tackling the COVID-19 pandemic.

PRACE (Partnership for Advanced Computing in Europe), an international not-for-profit association that brings together the five largest European supercomputing centers and involves 26 European countries, has allocated more than half a billion core hours to computer simulations to fight the COVID-19 pandemic. Alongside experiments, these simulations are a pillar of research to assess the risks of different scenarios and investigate mitigation strategies. While the world deals with the subsequent waves of the pandemic, we present a reflection on the use of urgent supercomputing for global societal challenges and crisis management.

Brain research challenges supercomputing.

Big data obtained from unraveling human brain structure raise processing demands.

Facile Fabrication of Hybrid Carbon Nanotube Sensors by Laser Direct Transfer.

Ammonia is one of the most frequently produced chemicals in the world, and thus, reliable measurements of different NH3 concentrations are critical for a variety of industries, among which are the agricultural and healthcare sectors. The currently available technologies for the detection of NH3 provide accurate identification; however, they are limited by size, portability, and fabrication cost. Therefore, in this work, we report the laser-induced forward transfer (LIFT) of single-walled carbon nanotubes (SWCNTs) decorated with tin oxide nanoparticles (SnO2 NPs), which act as sensitive materials in chemiresistive NH3 sensors. We demonstrate that the LIFT-fabricated sensors can detect NH3 at room temperature and have a response time of 13 s (for 25 ppm NH3). In addition, the laser-fabricated sensors are fully reversible when exposed to multiple cycles of NH3 and have an excellent theoretical limit of detection of 24 ppt.

Surface Analysis of Perovskite Oxynitride Thin Films as Photoelectrodes for Solar Water Splitting.

Perovskite oxynitride semiconductors have attracted huge interest recently as promising photoelectrode materials for photoelectrochemical (PEC) water splitting. Depicted by, the extensive studies of the PEC activity of oxynitride powder-based photoelectrodes and/or deposited thin-film electrodes. High-crystalline-quality, oxynitride thin films grown by physical vapor deposition are ideal model systems to study the fundamental physical and chemical properties of the surface of these materials, including their evolution. In this work, using a combination of high-sensitivity low-energy ion scattering (LEIS) and X-ray photoelectron spectroscopy (XPS), we monitor surface evolution of LaTiOxNy (LTON) and CaNbOxNy (CNON) thin films before and after the PEC characterizations. The as-prepared epitaxial LTON films show a preferential LaO termination at the surface layers, followed by a Ti-enriched subsurface. Whereas, the polycrystalline CNON thin films exhibit a non-uniform surface, with a mixed surface termination and a significant Ca-segregated subsurface. After the PEC characterizations, additional precipitated LaO species are found on the outer surface of the LTON epitaxial films. However, no significant surface change is observed on the polycrystalline CNON films by LEIS. The XPS analysis shows, an increase of the oxidized Ti and Nb cations (Ti4+ and Nb5+) after the PEC reaction in the LTON and CNON films, respectively. The initial drops in photocurrent for the LTON and CNON films are attributed to the changes in the surface chemical status. This work provides insight into the surface characteristics and evolution of LTON and CNON oxynitride thin films as photoelectrodes for PEC applications.

Modeling the spread of COVID-19 in Germany: Early assessment and possible scenarios.

The novel coronavirus (SARS-CoV-2), identified in China at the end of December 2019 and causing the disease COVID-19, has meanwhile led to outbreaks all over the globe with about 2.2 million confirmed cases and more than 150,000 deaths as of April 17, 2020. In this work, mathematical models are used to reproduce data of the early evolution of the COVID-19 outbreak in Germany, taking into account the effect of actual and hypothetical non-pharmaceutical interventions. Systems of differential equations of SEIR type are extended to account for undetected infections, stages of infection, and age groups. The models are calibrated on data until April 5. Data from April 6 to 14 are used for model validation. We simulate different possible strategies for the mitigation of the current outbreak, slowing down the spread of the virus and thus reducing the peak in daily diagnosed cases, the demand for hospitalization or intensive care units admissions, and eventually the number of fatalities. Our results suggest that a partial (and gradual) lifting of introduced control measures could soon be possible if accompanied by further increased testing activity, strict isolation of detected cases, and reduced contact to risk groups.

Effects of ultrasonic reactor design on sewage sludge disintegration.

The impact of ultrasound (US) reactor design on cavitation intensity distribution and disintegration efficiency was studied for sewage sludge pre-treatment, using a US flatbed reactor of variable reaction chamber height (RCH, 20-100 mm). Mapping of cavitation intensity and treatment effects was conducted using (i) hydrophone measurements, (ii) aluminum foil tests, and (iii) soluble chemical oxygen demand (COD) analyses. The overall disintegration efficiency was evaluated based on average COD solubilization. The impact of flow on treatment (in)homogeneity was additionally examined using computational fluid dynamics (CFD). Results of all measurement techniques suggest that small RCHs (20 mm, for instance) enable uniform and intense treatments, while large RCHs, which are subjected to strong sound wave attenuation, entail inhomogeneous treatments where large fractions of substrate are no longer exposed to notable cavitation activity. For instance, COD solubilization (relative to alkaline hydrolysis) measured in the channel center dropped from 6.4% to zero as RCH widened from 20 mm to 100 mm. Flow-through sonication further aggravates treatment inhomogeneity due to the high flow rates in the low-cavitation channel centers. Overall disintegration efficiency declined with increasing RCH, showing a drop in average COD solubilization by 73% from RCH = 20 mm to RCH = 100 mm. The drop correlated with average cavitation noise levels (R2 = 0.82), indicating that hydrophone measurements may be a suitable tool for US reactor design optimization. Overall, results suggest that reactor geometry has a critical impact on both treatment (in)homogeneity and treatment efficiency and that equal specific energy inputs do not imply equal US treatments.

Black-Si as a Photoelectrode.

The fabrication and characterization of photoanodes based on black-Si (b-Si) are presented using a photoelectrochemical cell in NaOH solution. B-Si was fabricated by maskless dry plasma etching and was conformally coated by tens-of-nm of TiO2 using atomic layer deposition (ALD) with a top layer of CoO x cocatalyst deposited by pulsed laser deposition (PLD). Low reflectivity R < 5 % of b-Si over the entire visible and near-IR ( λ < 2   µ m) spectral range was favorable for the better absorption of light, while an increased surface area facilitated larger current densities. The photoelectrochemical performance of the heterostructured b-Si photoanode is discussed in terms of the n-n junction between b-Si and TiO2.

Examining the surface evolution of LaTiOxNy an oxynitride solar water splitting photocatalyst.

LaTiOxNy oxynitride thin films are employed to study the surface modifications at the solid-liquid interface that occur during photoelectrocatalytic water splitting. Neutron reflectometry and grazing incidence x-ray absorption spectroscopy were utilised to distinguish between the surface and bulk signals, with a surface sensitivity of 3 nm. Here we show, contrary to what is typically assumed, that the A cations are active sites that undergo oxidation at the surface as a consequence of the water splitting process. Whereas, the B cations undergo local disordering with the valence state remaining unchanged. This surface modification reduces the overall water splitting efficiency, but is suppressed when the oxynitride thin films are decorated with a co-catalyst. With this example we present the possibilities of surface sensitive studies using techniques capable of operando measurements in water, opening up new opportunities for applications to other materials and for surface sensitive, operando studies of the water splitting process.

Systematic Material Study Reveals TiNb2 O7 as a Model Wide-Bandgap Photoanode Material for Solar Water Splitting.

This work reveals that photoanodes based on TiNb2 O7 (TNO) powder show remarkable water-oxidation properties including nearly ideal charge-transfer and charge-injection efficiencies. Furthermore, using a simplified photoanode construction and carefully surveying the structural and morphological characteristics of oriented and polycrystalline thin films and powder-based samples revealed that the water-splitting kinetics of TNO is negligibly effected by surface morphology; instead, internal grain boundaries likely play a driving role. The current powder-based TNO photoanodes exhibit ideal water-oxidation kinetics and oxidize water at minimal applied biases under illumination; consequently, TNO exhibits an early onset photocurrent voltage (0.4 V vs. RHE) that rivals that of other state-of-the-art photoanode materials.

Assessment of sonotrode and tube reactors for ultrasonic pre-treatment of two different sewage sludge types.

The effectiveness of tube and sonotrode reactors for the sonication of sewage sludge under identical conditions was compared for the first time. Despite the considerable structural differences, sonication with each ultrasonic reactor led to an accelerated degradation rate and an increased methane production within the first five days for the majority of the sewage sludge samples tested. On closer examination, however, it becomes clear that the investigated sonication systems are not equally suitable for the substrates considered. While the use of a sonotrode proved to be particularly advantageous for the treatment of waste activated sludge (+25% methane yield at 300 kJ/kgTS), the use of a 2-inch tube reactor achieved the highest enhancement for low-intensity sonication in digested sludge (+22% methane yield at 300 kJ/kgTS). With increasing energy input, more chemical oxygen demand was solubilized, but this did not result in an increase in methane yield for all samples. Sonication of waste activated sludge led to a significant reduction in viscosity of up to 50%, and a reduction of up to 60% was observed after sonication of digested sludge with low energy inputs. The study, therefore, demonstrates that the choice of the most suitable sonication system essentially depends on the properties of the sludge to be sonicated.

Geometrical Frustration and Planar Triangular Antiferromagnetism in Quasi-Three-Dimensional Artificial Spin Architecture.

We present a realization of highly frustrated planar triangular antiferromagnetism achieved in a quasi-three-dimensional artificial spin system consisting of monodomain Ising-type nanomagnets lithographically arranged onto a deep-etched silicon substrate. We demonstrate how the three-dimensional spin architecture results in the first direct observation of long-range ordered planar triangular antiferromagnetism, in addition to a highly disordered phase with short-range correlations, once competing interactions are perfectly tuned. Our work demonstrates how escaping two-dimensional restrictions can lead to new types of magnetically frustrated metamaterials.

The Human Brain Project-Synergy between neuroscience, computing, informatics, and brain-inspired technologies.

The Human Brain Project (HBP) is a European flagship project with a 10-year horizon aiming to understand the human brain and to translate neuroscience knowledge into medicine and technology. To achieve such aims, the HBP explores the multilevel complexity of the brain in space and time; transfers the acquired knowledge to brain-derived applications in health, computing, and technology; and provides shared and open computing tools and data through the HBP European brain research infrastructure. We discuss how the HBP creates a transdisciplinary community of researchers united by the quest to understand the brain, with fascinating perspectives on societal benefits.