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- ItemAtomically controlled CVD processing of group IV semiconductors for ultra-large-scale integrations(Bristol : IOP Publishing, 2012) Murota, Junichi; Sakuraba, Masao; Tillack, BerndOne of the main requirements for ultra-large-scale integrations (ULSIs) is atomic-order control of process technology. Our concept of atomically controlled processing is based on atomic-order surface reaction control by CVD. By ultraclean low-pressure CVD using SiH4 and GeH4 gases, high-quality low-temperature epitaxial growth of Si1−xGex (100) (x=0–1) with atomically flat surfaces and interfaces on Si(100) is achieved. Self-limiting formation of 1–3 atomic layers of group IV or related atoms in the thermal adsorption and reaction of hydride gases on Si1-xGex (100) are generalized based on the Langmuir-type model. By the Si epitaxial growth on top of the material already-formed on Si(100), N, B and C atoms are confined within about a 1 nm thick layer. In Si cap layer growth on the P atomic layer formed on Si1−xGex (100), segregation of P atoms is suppressed by using Si2H6 instead of SiH4 at a low temperature of 450 °C. Heavy C atomic-layer doping suppresses strain relaxation as well as intermixing between Si and Ge at the Si1−xGex/Si heterointerface. It is confirmed that higher carrier concentration and higher carrier mobility are achieved by atomic-layer doping. These results open the way to atomically controlled technology for ULSIs.
- ItemBoundary conditions for electrochemical interfaces(Bristol : IOP Publishing, 2017) Landstorfer, ManuelConsistent boundary conditions for electrochemical interfaces, which cover double layer charging, pseudo-capacitive effects and transfer reactions, are of high demand in electrochemistry and adjacent disciplines. Mathematical modeling and optimization of electrochemical systems is a strongly emerging approach to reduce cost and increase efficiency of super-capacitors, batteries, fuel cells, and electro-catalysis. However, many mathematical models which are used to describe such systems lack a real predictive value. Origin of this shortcoming is the usage of oversimplified boundary conditions. In this work we derive the boundary conditions for some general electrode-electrolyte interface based on non-equilibrium thermodynamics for volumes and surfaces. The resulting equations are widely applicable and cover also tangential transport. The general framework is then applied to a specific material model which allows the deduction of a current-voltage relation and thus a comparison to experimental data. Some simplified 1D examples show the range of applicability of the new approach.
- ItemForce microscopy of layering and friction in an ionic liquid(Bristol : IOP Publishing, 2014) Hoth, Judith; Hausen, Florian; Müser, Martin H.; Bennewitz, RolandThe mechanical properties of the ionic liquid 1-butyl-1-methylpyrrolidinium tris(pentafluoroethyl) trifluorophosphate ([Py1,4][FAP]) in confinement between a SiOx and a Au(1 1 1) surface are investigated by means of atomic force microscopy (AFM) under electrochemical control. Up to 12 layers of ion pairs can be detected through force measurements while approaching the tip of the AFM to the surface. The particular shape of the force versus distance curve is explained by a model for the interaction between tip, gold surface and ionic liquid, which assumes an exponentially decaying oscillatory force originating from bulk liquid density correlations. Jumps in the tip–sample distance upon approach correspond to jumps of the compliant force sensor between branches of the oscillatory force curve. Frictional force between the laterally moving tip and the surface is detected only after partial penetration of the last double layer between tip and surface.
- ItemImproved Capacitive Deionization Performance of Mixed Hydrophobic / Hydrophilic Activated Carbon Electrodes(Bristol : IOP Publishing, 2016) Aslan, Mesut; Zeiger, Marco; Jäckel, Nicolas; Grobelsek, Ingrid; Weingarth, Daniel; Presser, VolkerCapacitive deionization (CDI) is a promising salt removal technology with high energy efficiency when applied to low molar concentration aqueous electrolytes. As an interfacial process, ion electrosorption during CDI operation is sensitive to the pore structure and the total pore volume of carbon electrodes limit the maximum salt adsorption capacity (SAC). Thus, activation of carbons as a widely used method to enhance the porosity of a material should also be highly attractive for improving SAC values. In our study, we use easy-to-scale and facile-to-apply CO2 activation at temperatures between 950 °C and 1020 °C to increase the porosity of commercially available activated carbon. While the pore volume and surface area can be significantly increased up to 1.51 cm3/g and 2113 m2/g, this comes at the expense of making the carbon more hydrophobic. We present a novel strategy to still capitalize the improved pore structure by admixing as received (more hydrophilic) carbon with CO2 treated (more hydrophobic) carbon for CDI electrodes without using membranes. This translates in an enhanced charge storage ability in high and low molar concentrations (1 M and 5 mM NaCl) and significantly improved CDI performance (at 5 mM NaCl). In particular, we obtain stable CDI performance at 0.86 charge efficiency with 13.1 mg/g SAC for an optimized 2:1 mixture (by mass).
- ItemNational contributions for decarbonizing the world economy in line with the G7 agreement(Bristol : IOP Publishing, 2016) du Pont, Yann Robiou; Jeffery, M. Louise; Gütschow, Johannes; Christoff, Peter; Meinshausen, MalteIn June 2015, the G7 agreed to two global mitigation goals: 'a decarbonization of the global economy over the course of this century' and 'the upper end of the latest Intergovernmental Panel on Climate Change (IPCC) recommendation of 40%–70% reductions by 2050 compared to 2010'. These IPCC recommendations aim to preserve a likely (>66%) chance of limiting global warming to 2 °C but are not necessarily consistent with the stronger ambition of the subsequent Paris Agreement of 'holding the increase in the global average temperature to well below 2 °C above pre-industrial levels and to pursue efforts to limit the temperature increase to 1.5 °C above pre-industrial levels'. The G7 did not specify global or national emissions scenarios consistent with its own agreement. Here we identify global cost-optimal emissions scenarios from Integrated Assessment Models that match the G7 agreement. These scenarios have global 2030 emissions targets of 11%–43% below 2010, global net negative CO2 emissions starting between 2056 and 2080, and some exhibit net negative greenhouse gas emissions from 2080 onwards. We allocate emissions from these global scenarios to countries according to five equity approaches representative of the five equity categories presented in the Fifth Assessment Report of the IPCC (IPCCAR5): 'capability', 'equality', 'responsibility-capability-need', 'equal cumulative per capita' and 'staged approaches'. Our results show that G7 members' Intended Nationally Determined Contribution (INDCs) mitigation targets are in line with a grandfathering approach but lack ambition to meet various visions of climate justice. The INDCs of China and Russia fall short of meeting the requirements of any allocation approach. Depending on how their INDCs are evaluated, the INDCs of India and Brazil can match some equity approaches evaluated in this study.
- ItemFabrication of metal nanoparticle arrays by controlled decomposition of polymer particles(Bristol : IOP Publishing, 2013) Brodoceanu, Daniel; Fang, Cheng; Voelcker, Nicolas Hans; Bauer, Christina T.; Wonn, Anne; Kroner, Elmar; Arzt, Eduard; Kraus, TobiasWe report a novel fabrication method for ordered arrays of metal nanoparticles that exploits the uniform arrangement of polymer beads deposited as close-packed monolayers. In contrast to colloidal lithography that applies particles as masks, we used thermal decomposition of the metal-covered particles to precisely define metal structures. Large arrays of noble metal (Au, Ag, Pt) nanoparticles were produced in a three-step process on silicon, fused silica and sapphire substrates, demonstrating the generality of this approach. Polystyrene spheres with diameters ranging between 110 nm and 1 µm were convectively assembled into crystalline monolayers, coated with metal and annealed in a resistive furnace or using an ethanol flame. The thermal decomposition of the polymer microspheres converted the metal layer into particles arranged in hexagonal arrays that preserved the order of the original monolayer. Both the particle size and the interparticle distance were adjusted via the thickness of the metal coating and the sphere diameter, respectively.
- ItemFabrication of silicon nanowire arrays by near-field laser ablation and metal-assisted chemical etching(Bristol : IOP Publishing, 2016) Brodoceanu, Daniel; Alhmoud, Hashim Z.; Elnathan, Roey; Delalat, Bahman; Voelcker, Nicolas H.; Kraus, TobiasWe present an elegant route for the fabrication of ordered arrays of vertically-aligned silicon nanowires with tunable geometry at controlled locations on a silicon wafer. A monolayer of transparent microspheres convectively assembled onto a gold-coated silicon wafer acts as a microlens array. Irradiation with a single nanosecond laser pulse removes the gold beneath each focusing microsphere, leaving behind a hexagonal pattern of holes in the gold layer. Owing to the near-field effects, the diameter of the holes can be at least five times smaller than the laser wavelength. The patterned gold layer is used as catalyst in a metal-assisted chemical etching to produce an array of vertically-aligned silicon nanowires. This approach combines the advantages of direct laser writing with the benefits of parallel laser processing, yielding nanowire arrays with controlled geometry at predefined locations on the silicon surface. The fabricated VA-SiNW arrays can effectively transfect human cells with a plasmid encoding for green fluorescent protein.
- ItemBa termination of Ge(001) studied with STM(Bristol : IOP Publishing, 2015) Koczorowski, W.; Grzela, T.; Radny, M.W.; Schofield, S.R.; Capellini, G.; Czajka, R.; Schroeder, T.; Curson, N.J.We use controlled annealing to tune the interfacial properties of a sub-monolayer and monolayer coverages of Ba atoms deposited on Ge(001), enabling the generation of either of two fundamentally distinct interfacial phases, as revealed by scanning tunneling microscopy. Firstly we identify the two key structural phases associated with this adsorption system, namely on-top adsorption and surface alloy formation, by performing a deposition and annealing experiment at a coverage low enough (~0.15 ML) that isolated Ba-related features can be individually resolved. Subsequently we investigate the monolayer coverage case, of interest for passivation schemes of future Ge based devices, for which we find that the thermal evaporation of Ba onto a Ge(001) surface at room temperature results in on-top adsorption. This separation (lack of intermixing) between Ba and Ge layers is retained through successive annealing steps to temperatures of 470, 570, 670 and 770 K although a gradual ordering of the Ba layer is observed at 570 K and above, accompanied by a decrease in Ba layer density. Annealing above 770 K produces the 2D surface alloy phase accompanied by strain relief through monolayer height trench formation. An annealing temperature of 1070 K sees a further change in surface morphology but retention of the 2D surface alloy characteristic. These results are discussed in view of their possible implications for future semiconductor integrated circuit technology.
- ItemMicrostructure evolution during annealing of an SPD- processed supersaturated Cu – 3 at.% Ag alloy(Bristol : IOP Publishing, 2014) Gubicza, J.; Hegedűs, Z.; Lábár, J.L.; Sarma, V.S.; Kauffmann, A.; Freudenberger, J.Supersaturated Cu-3 at.% Ag alloy was processed by rolling at liquid nitrogen temperature and subsequent annealing at 623 K up to 20 min. It was found that after annealing, an inhomogeneous solute atom distribution developed, since the Ag particles with small size and/or large specific interfacial energy were dissolved due to the Gibbs-Thomson effect. In the region where the solute concentration increased, a high dislocation density was retained in the Cu matrix even after annealing, while in the region where the Ag solute content did not increase, the dislocation density decreased by more than one order of magnitude. Therefore, in the cryorolled and annealed samples, heterogeneous microstructures were developed where both the dislocation density and the solute concentration varied considerably.
- ItemExtreme fire events are related to previous-year surface moisture conditions in permafrost-underlain larch forests of Siberia(Bristol : IOP Publishing, 2012) Forkel, Matthias; Thonicke, Kirsten; Beer, Christian; Cramer, Wolfgang; Bartalev, Sergey; Schmullius, ChristianeWildfires are a natural and important element in the functioning of boreal forests. However, in some years, fires with extreme spread and severity occur. Such severe fires can degrade the forest, affect human values, emit huge amounts of carbon and aerosols and alter the land surface albedo. Usually, wind, slope and dry air conditions have been recognized as factors determining fire spread. Here we identify surface moisture as an additional important driving factor for the evolution of extreme fire events in the Baikal region. An area of 127 000 km2 burned in this region in 2003, a large part of it in regions underlain by permafrost. Analyses of satellite data for 2002–2009 indicate that previous-summer surface moisture is a better predictor for burned area than precipitation anomalies or fire weather indices for larch forests with continuous permafrost. Our analysis advances the understanding of complex interactions between the atmosphere, vegetation and soil, and how coupled mechanisms can lead to extreme events. These findings emphasize the importance of a mechanistic coupling of soil thermodynamics, hydrology, vegetation functioning, and fire activity in Earth system models for projecting climate change impacts over the next century.