252 research outputs found

    German commercial policy and party politics, 1890-1903 /

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    Networkability in the Health Care Sector - Necessity, Measurement and Systematic Development as the Prerequisites for Increasing the Operational Efficiency of Administrative Processes

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    The health care sector is characterised by a low division of labour and annually rising costs. In order to increase effectiveness and efficiency, other sectors have implemented a high division of labour and extensive networking, in particular through the use of IT. In the health care sector, however, networking is only progressing at a very slow pace and not along a wide front. While initial approaches to networking already exist at the technical level or for the purpose of process optimisation, holistic approaches are missing. In this article, the authors first show how a generic, holistic framework for designing networked structures can be transferred to the health care sector. Then the concept of networkability and its design objects are introduced. In order to assess networkability, the use of development levels for design objects is proposed so that a maturity stage model can be derived on this basis for the various players in the health care sector. Thereafter the results of an expert workshop regarding the main design objects which determine networkability in the health care sector are presented. The article concludes with a description of the procedure for validating and further developing the findings obtained

    Success Factors of Application Integration: An Exploratory Analysis

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    The increased deployment of commercial off-the-shelf (COTS) applications creates application integration challenges. However, very few articles focus on application integration success. That is why we first analyze these contributions and derive success factor candidates (SFCs). In addition, contributions dealing with problems and risks of application integration and related research fields are examined—as they allow for the derivation of further SFCs. In total twenty-six SFCs are collected. A factor analysis is conducted to examine interrelations between SFCs. It yields seven success factor groups, e.g., architecture management, IT/business alignment, or use of methods. In a second step, an exploratory analysis is conducted to examine the impact of these SFCs on various success indicators of application integration. These success indicators were defined beforehand by analyzing theories for information system (IS) success. As a result of the exploratory analysis, twenty-seven hypotheses are proposed. These hypotheses need to be corroborated in a future confirmatory study

    Good Intentions: Adaptive Parameter Management via Intent Signaling

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    Parameter management is essential for distributed training of large machine learning (ML) tasks. Some ML tasks are hard to distribute because common approaches to parameter management can be highly inefficient. Advanced parameter management approaches -- such as selective replication or dynamic parameter allocation -- can improve efficiency, but to do so, they typically need to be integrated manually into each task's implementation and they require expensive upfront experimentation to tune correctly. In this work, we explore whether these two problems can be avoided. We first propose a novel intent signaling mechanism that integrates naturally into existing ML stacks and provides the parameter manager with crucial information about parameter accesses. We then describe AdaPM, a fully adaptive, zero-tuning parameter manager based on this mechanism. In contrast to prior systems, this approach separates providing information (simple, done by the task) from exploiting it effectively (hard, done automatically by AdaPM). In our experimental evaluation, AdaPM matched or outperformed state-of-the-art parameter managers out of the box, suggesting that automatic parameter management is possible

    Structural and Chemical Properties of NiOₓ Thin Films: Oxygen Vacancy Formation in O₂ Atmosphere

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    NiOₓ films on Si(111) were put in contact with oxygen at elevated temperatures. During heating and cooling in oxygen atmosphere Near Ambient Pressure (NAP)‐XPS and ‐XAS and work function (WF) measurements reveal the creation and replenishing of oxygen vacancies in dependence of temperature. Oxygen vacancies manifest themselves as a distinct O1s feature at 528.9 eV on the low binding energy side of the main NiO peak as well as by a distinct deviation of the Ni2p₃/₂ spectral features from the typical NiO spectra. DFT calculations reveal that the presence of oxygen vacancies leads to a charge redistribution and altered bond lengths of the atoms surrounding the vacancies causing the observed spectral changes. Furthermore, we observed that a broadening of the lowest energy peak in the O K‐edge spectra can be attributed to oxygen vacancies. In the presence of oxygen vacancies, the WF is lowered by 0.1 eV

    Triply bonded pancake π-dimers stabilized by tetravalent actinides

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    Aromatic π-stacking is a weakly attractive, noncovalent interaction often found in biological macromolecules and synthetic supramolecular chemistry. The weak nondirectional nature of π-stacking can present challenges in the design of materials owing to their weak, nondirectional nature. However, when aromatic π-systems contain an unpaired electron, stronger attraction involving face-to-face π-orbital overlap is possible, resulting in covalent so-called “pancake” bonds. Two-electron, multicenter single pancake bonds are well known, whereas four-electron double pancake bonds are rare. Higher-order pancake bonds have been predicted, but experimental systems are unknown. Here, we show that six-electron triple pancake bonds can be synthesized by a 3-fold reduction of hexaazatrinaphthylene (HAN) and subsequent stacking of the [HAN]3– triradicals. Our analysis reveals a multicenter covalent triple pancake bond consisting of a σ-orbital and two equivalent π-orbitals. An electrostatic stabilizing role is established for the tetravalent thorium and uranium ions in these systems. We also show that the electronic absorption spectrum of the triple pancake bonds closely matches computational predictions, providing experimental verification of these unique interactions. The discovery of conductivity in thin films of triply bonded π-dimers presents new opportunities for the discovery of single-component molecular conductors and other spin-based molecular materials

    Surface Electron-Hole Rich Species Active in the Electrocatalytic Water Oxidation.

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    Iridium and ruthenium and their oxides/hydroxides are the best candidates for the oxygen evolution reaction under harsh acidic conditions owing to the low overpotentials observed for Ru- and Ir-based anodes and the high corrosion resistance of Ir-oxides. Herein, by means of cutting edge operando surface and bulk sensitive X-ray spectroscopy techniques, specifically designed electrode nanofabrication and ab initio DFT calculations, we were able to reveal the electronic structure of the active IrOx centers (i.e., oxidation state) during electrocatalytic oxidation of water in the surface and bulk of high-performance Ir-based catalysts. We found the oxygen evolution reaction is controlled by the formation of empty Ir 5d states in the surface ascribed to the formation of formally IrV species leading to the appearance of electron-deficient oxygen species bound to single iridium atoms (Ό1-O and Ό1-OH) that are responsible for water activation and oxidation. Oxygen bound to three iridium centers (Ό3-O) remains the dominant species in the bulk but do not participate directly in the electrocatalytic reaction, suggesting bulk oxidation is limited. In addition a high coverage of a Ό1-OO (peroxo) species during the OER is excluded. Moreover, we provide the first photoelectron spectroscopic evidence in bulk electrolyte that the higher surface-to-bulk ratio in thinner electrodes enhances the material usage involving the precipitation of a significant part of the electrode surface and near-surface active species

    Dynamics at polarized carbon dioxide-iron oxyhydroxide interfaces unveil the origin of multicarbon product formation

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    Surface-sensitive ambient pressure X-ray photoelectron spectroscopy and near-edge X-ray absorption fine structure spectroscopy combined with an electrocatalytic reactivity study, multilength-scale electron microscopy, and theoretical modeling provide insights into the gas-phase selective reduction of carbon dioxide to isopropanol on a nitrogen-doped carbon-supported iron oxyhydroxide electrocatalyst. Dissolved atomic carbon forms at relevant potentials for carbon dioxide reduction from the reduction of carbon monoxide chemisorbed on the surface of the ferrihydrite-like phase. Theoretical modeling reveals that the ferrihydrite structure allows vicinal chemisorbed carbon monoxide in the appropriate geometrical arrangement for coupling. Based on our observations, we suggest a mechanism of three-carbon-atom product formation, which involves the intermediate formation of atomic carbon that undergoes hydrogenation in the presence of hydrogen cations upon cathodic polarization. This mechanism is effective only in the case of thin ferrihydrite-like nanostructures coordinated at the edge planes of the graphitic support, where nitrogen edge sites stabilize these species and lower the overpotential for the reaction. Larger ferrihydrite-like nanoparticles are ineffective for electron transport

    In situ observations of the atomistic mechanisms of Ni catalyzed low temperature graphene growth.

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    The key atomistic mechanisms of graphene formation on Ni for technologically relevant hydrocarbon exposures below 600 °C are directly revealed via complementary in situ scanning tunneling microscopy and X-ray photoelectron spectroscopy. For clean Ni(111) below 500 °C, two different surface carbide (Ni2C) conversion mechanisms are dominant which both yield epitaxial graphene, whereas above 500 °C, graphene predominantly grows directly on Ni(111) via replacement mechanisms leading to embedded epitaxial and/or rotated graphene domains. Upon cooling, additional carbon structures form exclusively underneath rotated graphene domains. The dominant graphene growth mechanism also critically depends on the near-surface carbon concentration and hence is intimately linked to the full history of the catalyst and all possible sources of contamination. The detailed XPS fingerprinting of these processes allows a direct link to high pressure XPS measurements of a wide range of growth conditions, including polycrystalline Ni catalysts and recipes commonly used in industrial reactors for graphene and carbon nanotube CVD. This enables an unambiguous and consistent interpretation of prior literature and an assessment of how the quality/structure of as-grown carbon nanostructures relates to the growth modes.L.L.P. acknowledges funding from Area di Ricerca Scientifica e Tecnologica of Trieste and from MIUR through Progetto Strategico NFFA. C.A. acknowledges support from CNR through the ESF FANAS project NOMCIS. C.A. and C.C. acknowledge financial support from MIUR (PRIN 2010-2011 nÂș 2010N3T9M4). S.B. acknowledges funding from ICTP TRIL program. S.H. acknowledges funding from ERC grant InsituNANO (n°279342). R.S.W. acknowledges funding from EPSRC (Doctoral training award), and the Nano Science & Technology Doctoral Training Centre Cambridge (NanoDTC). The help of C. Dri and F. Esch (design) and P. Bertoch and F. Salvador (manufacturing) in the realization of the high temperature STM sample holder is gratefully acknowledged. We acknowledge the Helmholtz-Zentrum-Berlin Electron storage ring BESSY II for provision of synchrotron radiation at the ISISS beamline and we thank the BESSY staff for continuous support of our experiments.This is the accepted manuscript. The final version is available from ACS at http://pubs.acs.org/doi/abs/10.1021/nn402927q
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