Enhancing composition control of alloy nanoparticles from gas aggregation source by in operando optical emission spectroscopy

The use of multicomponent targets allows the gas‐phase synthesis of a large variety of alloy nanoparticles (NPs) via gas aggregation sources. However, the redeposition of sputtered material impacts the composition of alloy NPs, as demonstrated here for the case of AgAu alloy NPs. To enable NPs with tailored Au fractions, in operando control over the composition of the NPs is in high demand. We suggest the use of optical emission spectroscopy as a versatile diagnostic tool to determine and control the composition of the NPs. A strong correlation between operating pressure, intensity ratio of Ag and Au emission lines, and the obtained NP compositions is observed. This allows precise in operando control of alloy NP composition obtained from multicomponent targets

In Situ Laser Light Scattering for Temporally and Locally Resolved Studies on Nanoparticle Trapping in a Gas Aggregation Source

Gas phase synthesis of nanoparticles (NPs) via magnetron sputtering in a gas aggregation source (GAS) has become a well-established method since its conceptualization three decades ago. NP formation is commonly described in terms of nucleation, growth, and transport alongside the gas stream. However, the NP formation and transport involve complex non-equilibrium processes, which are still the subject of investigation. The development of in situ investigation techniques such as UV–Vis spectroscopy and small angle X-ray scattering enabled further insights into the dynamic processes inside the GAS and have recently revealed NP trapping at different distances from the magnetron source. The main drawback of these techniques is their limited spatial resolution. To understand the spatio-temporal behavior of NP trapping, an in situ laser light scattering technique is applied in this study. By this approach, silver NPs are made visible inside the GAS with good spatial and temporal resolution. It is found that the argon gas pressure, as well as different gas inlet configurations, have a strong impact on the trapping behavior of NPs inside the GAS. The different gas inlet configurations not only affect the trapping of NPs, but also the size distribution and deposition rate of NPs

Enhancing Reliability of Studies on Single Filament Memristive Switching via an Unconventional cAFM Approach

Memristive devices are highly promising for implementing neuromorphic functionalities in future electronic hardware, and direct insights into memristive phenomena on the nanoscale are of fundamental importance to reaching this. Conductive atomic force microscopy (cAFM) has proven to be an essential tool for probing memristive action locally on the nanoscale, but the significance of the acquired data frequently suffers from the nonlocality associated with the thermal drift of the tip in ambient conditions. Furthermore, comparative studies of different configurations of filamentary devices have proven to be difficult, because of an immanent variability of the filament properties between different devices. Herein, these problems are addressed by constraining the memristive action directly at the apex of the probe through functionalization of a cAFM tip with an archetypical memristive stack, which is comprised of Ag/Si3N4. The design of such functionalized cantilevers (entitled here as "memtips") allowed the capture of the long-term intrinsic current response, identifying temporal correlations between switching events, and observing emerging spiking dynamics directly at the nanoscale. Utilization of an identical memtip for measurements on different counter electrodes made it possible to directly compare the impact of different device configurations on the switching behavior of the same filament. Such an analytical approach in ambient conditions will pave the way towards a deeper understanding of filamentary switching phenomena on the nanoscale

Anomalous Surface Compositions of Stoichiometric Mixed Oxide Compounds

The surface compositions of bulk mixed metal oxides stoichiometric vanadate and molybdate compounds have been systematically examined, for the first time, by combined synchroton-based depth-resolved XPS profile analysis, conventional XPS and LEIS spectroscopy. The outer surfaces of many, but not all, of the bulk mixed vanadates and molybdates tend to be enriched with surface VOx and MoOx species approaching monolayer coverage. Furthermore, this surface enrichment phenomenon can be dramatically enhanced in the presence of minor amount of alkali impurities. These new findings have significant implications for the fundamental understanding of how bulk mixed oxide materials function in numerous technical applications.Fil: Merzlikin, Sergiy V. . Ruhr-Universitt Bochum, Lehrstuhl fr Technische Chemie; AlemaniaFil: Tolkachev, Nikolay N. . Russian Academy of Sciences, N. D. Zelinsky Institute of Organic Chemistry; RusiaFil: Briand, Laura Estefania. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico La Plata. Centro de Investigación y Desarrollo en Ciencias Aplicadas; ArgentinaFil: Strunskus,Thomas . Ruhr-Universitt Bochum, Lehrstuhl Physikalische Chemie; AlemaniaFil: Wöll, Christof. Ruhr-Universitt Bochum, Lehrstuhl Physikalische Chemie; AlemaniaFil: Wachs, Israel E.. Lehigh University Bethlehem, Department of Chemical Engineering, Operando Molecular Spectroscopy and Catalysis Laboratory; Estados UnidosFil: Grüenert, Wolfgang . Ruhr-Universitt Bochum, Lehrstuhl fr Technische Chemie; Alemani

Anomalous Surface Compositions of Stoichiometric Mixed Oxide Compounds

The surface compositions of bulk mixed metal oxides stoichiometric vanadate and molybdate compounds have been systematically examined, for the first time, by combined synchroton-based depth-resolved XPS profile analysis, conventional XPS and LEIS spectroscopy. The outer surfaces of many, but not all, of the bulk mixed vanadates and molybdates tend to be enriched with surface VOx and MoOx species approaching monolayer coverage. Furthermore, this surface enrichment phenomenon can be dramatically enhanced in the presence of minor amount of alkali impurities. These new findings have significant implications for the fundamental understanding of how bulk mixed oxide materials function in numerous technical applications.Fil: Merzlikin, Sergiy V. . Ruhr-Universitt Bochum, Lehrstuhl fr Technische Chemie; AlemaniaFil: Tolkachev, Nikolay N. . Russian Academy of Sciences, N. D. Zelinsky Institute of Organic Chemistry; RusiaFil: Briand, Laura Estefania. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico La Plata. Centro de Investigación y Desarrollo en Ciencias Aplicadas; ArgentinaFil: Strunskus,Thomas . Ruhr-Universitt Bochum, Lehrstuhl Physikalische Chemie; AlemaniaFil: Wöll, Christof. Ruhr-Universitt Bochum, Lehrstuhl Physikalische Chemie; AlemaniaFil: Wachs, Israel E.. Lehigh University Bethlehem, Department of Chemical Engineering, Operando Molecular Spectroscopy and Catalysis Laboratory; Estados UnidosFil: Grüenert, Wolfgang . Ruhr-Universitt Bochum, Lehrstuhl fr Technische Chemie; Alemani

Anomalous Surface Compositions of Stoichiometric Mixed Oxide Compounds

The surface compositions of bulk mixed metal oxides stoichiometric vanadate and molybdate compounds have been systematically examined, for the first time, by combined synchroton-based depth-resolved XPS profile analysis, conventional XPS and LEIS spectroscopy. The outer surfaces of many, but not all, of the bulk mixed vanadates and molybdates tend to be enriched with surface VOx and MoOx species approaching monolayer coverage. Furthermore, this surface enrichment phenomenon can be dramatically enhanced in the presence of minor amount of alkali impurities. These new findings have significant implications for the fundamental understanding of how bulk mixed oxide materials function in numerous technical applications.Fil: Merzlikin, Sergiy V. . Ruhr-Universitt Bochum, Lehrstuhl fr Technische Chemie; AlemaniaFil: Tolkachev, Nikolay N. . Russian Academy of Sciences, N. D. Zelinsky Institute of Organic Chemistry; RusiaFil: Briand, Laura Estefania. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico La Plata. Centro de Investigación y Desarrollo en Ciencias Aplicadas; ArgentinaFil: Strunskus,Thomas . Ruhr-Universitt Bochum, Lehrstuhl Physikalische Chemie; AlemaniaFil: Wöll, Christof. Ruhr-Universitt Bochum, Lehrstuhl Physikalische Chemie; AlemaniaFil: Wachs, Israel E.. Lehigh University Bethlehem, Department of Chemical Engineering, Operando Molecular Spectroscopy and Catalysis Laboratory; Estados UnidosFil: Grüenert, Wolfgang . Ruhr-Universitt Bochum, Lehrstuhl fr Technische Chemie; Alemani

Tuning the Selectivity of Metal Oxide Gas Sensors with Vapor Phase Deposited Ultrathin Polymer Thin Films

Metal oxide gas sensors are of great interest for applications ranging from lambda sensors to early hazard detection in explosive media and leakage detection due to their superior properties with regard to sensitivity and lifetime, as well as their low cost and portability. However, the influence of ambient gases on the gas response, energy consumption and selectivity still needs to be improved and they are thus the subject of intensive research. In this work, a simple approach is presented to modify and increase the selectivity of gas sensing structures with an ultrathin polymer thin film. The different gas sensing surfaces, CuO, Al2O3/CuO and TiO2 are coated with a conformal 200 °C. The present study demonstrates possibilities for improving the properties of metal oxide gas sensors, which is very important in applications in fields such as medicine, security and food safety

From Au-Thiolate Chains to Thioether Sierpiński Triangles: The Versatile Surface Chemistry of 1,3,5-Tris(4-Mercaptophenyl)Benzene on Au(111)

Self-assembly of 1,3,5-tris(4-mercaptophenyl)benzene (TMB) – a three-fold symmetric, thiol functionalized aromatic molecule – was studied on Au(111) with the aim to realize extended Au-thiolate linked molecular architectures. The focus lay on resolving thermally activated structural and chemical changes by a combination of microscopy and spectroscopy. Thereby Scanning Tunneling Microscopy provided submolecularly resolved structural information, while the chemical state of sulfur was assessed by X-ray Photoelectron Spectroscopy. Directly after room temperature deposition only less well ordered structures were observed. Mild annealing promoted the first structural transition into ordered molecular chains, partly organized in homochiral molecular braids. Further annealing led to self-similar Sierpiński triangles, while annealing at even higher temperatures again resulted in mostly disordered structures. Both the irregular aggregates observed at room temperature and the chains were identified as metal-organic assemblies, whereby two out of the three intermolecular binding motifs are energetically equivalent according to Density Functional Theory simulations. The emergence of Sierpiński triangles is driven by a chemical transformation, i.e. the conversion of coordinative Au-thiolate to covalent thioether linkages, and can be further understood by Monte Carlo simulations. The great structural variance of TMB on Au(111) can on one hand be explained by the energetic equivalence of two binding motifs. On the other hand, the unexpected chemical transition even enhances the structural variance and results in thiol-derived covalent molecular architectures

Epileptic Seizure Detection on an Ultra-Low-Power Embedded RISC-V Processor Using a Convolutional Neural Network

The treatment of refractory epilepsy via closed-loop implantable devices that act on seizures either by drug release or electrostimulation is a highly attractive option. For such implantable medical devices, efficient and low energy consumption, small size, and efficient processing architectures are essential. To meet these requirements, epileptic seizure detection by analysis and classification of brain signals with a convolutional neural network (CNN) is an attractive approach. This work presents a CNN for epileptic seizure detection capable of running on an ultra-low-power microprocessor. The CNN is implemented and optimized in MATLAB. In addition, the CNN is also implemented on a GAP8 microprocessor with RISC-V architecture. The training, optimization, and evaluation of the proposed CNN are based on the CHB-MIT dataset. The CNN reaches a median sensitivity of 90% and a very high specificity over 99% corresponding to a median false positive rate of 6.8 s per hour. After implementation of the CNN on the microcontroller, a sensitivity of 85% is reached. The classification of 1 s of EEG data takes t=35 ms and consumes an average power of P≈140 μW. The proposed detector outperforms related approaches in terms of power consumption by a factor of 6. The universal applicability of the proposed CNN based detector is verified with recording of epileptic rats. This results enable the design of future medical devices for epilepsy treatment