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- ItemMicrofluidic colloid filtration([London] : Macmillan Publishers Limited, part of Springer Nature, 2016) Linkhorst, John; Beckmann, Torsten; Go, Dennis; Kuehne, Alexander J. C.; Wessling, MatthiasFiltration of natural and colloidal matter is an essential process in today’s water treatment processes. The colloidal matter is retained with the help of micro- and nanoporous synthetic membranes. Colloids are retained in a “cake layer” – often coined fouling layer. Membrane fouling is the most substantial problem in membrane filtration: colloidal and natural matter build-up leads to an increasing resistance and thus decreasing water transport rate through the membrane. Theoretical models exist to describe macroscopically the hydrodynamic resistance of such transport and rejection phenomena; however, visualization of the various phenomena occurring during colloid retention is extremely demanding. Here we present a microfluidics based methodology to follow filter cake build up as well as transport phenomena occuring inside of the fouling layer. The microfluidic colloidal filtration methodology enables the study of complex colloidal jamming, crystallization and melting processes as well as translocation at the single particle level.
- ItemManipulation of small particles at solid liquid interface: Light driven diffusioosmosis([London] : Macmillan Publishers Limited, part of Springer Nature, 2016) Feldmann, David; Maduar, Salim R.; Santer, Mark; Lomadze, Nino; Vinogradova, Olga I.; Santer, SvetlanaThe strong adhesion of sub-micron sized particles to surfaces is a nuisance, both for removing contaminating colloids from surfaces and for conscious manipulation of particles to create and test novel micro/nano-scale assemblies. The obvious idea of using detergents to ease these processes suffers from a lack of control: the action of any conventional surface-modifying agent is immediate and global. With photosensitive azobenzene containing surfactants we overcome these limitations. Such photo-soaps contain optical switches (azobenzene molecules), which upon illumination with light of appropriate wavelength undergo reversible trans-cis photo-isomerization resulting in a subsequent change of the physico-chemical molecular properties. In this work we show that when a spatial gradient in the composition of trans- and cis- isomers is created near a solid-liquid interface, a substantial hydrodynamic flow can be initiated, the spatial extent of which can be set, e.g., by the shape of a laser spot. We propose the concept of light induced diffusioosmosis driving the flow, which can remove, gather or pattern a particle assembly at a solid-liquid interface. In other words, in addition to providing a soap we implement selectivity: particles are mobilized and moved at the time of illumination, and only across the illuminated area.
- ItemThe sequence to hydrogenate coronene cations: A journey guided by magic numbers([London] : Macmillan Publishers Limited, part of Springer Nature, 2016) Cazaux, Stéphanie; Boschman, Leon; Rougeau, Nathalie; Reitsma, Geert; Hoekstra, Ronnie; Teillet-Billy, Dominique; Morisset, Sabine; Spaans, Marco; Schlathölter, ThomasThe understanding of hydrogen attachment to carbonaceous surfaces is essential to a wide variety of research fields and technologies such as hydrogen storage for transportation, precise localization of hydrogen in electronic devices and the formation of cosmic H2. For coronene cations as prototypical Polycyclic Aromatic Hydrocarbon (PAH) molecules, the existence of magic numbers upon hydrogenation was uncovered experimentally. Quantum chemistry calculations show that hydrogenation follows a site-specific sequence leading to the appearance of cations having 5, 11, or 17 hydrogen atoms attached, exactly the magic numbers found in the experiments. For these closed-shell cations, further hydrogenation requires appreciable structural changes associated with a high transition barrier. Controlling specific hydrogenation pathways would provide the possibility to tune the location of hydrogen attachment and the stability of the system. The sequence to hydrogenate PAHs, leading to PAHs with magic numbers of H atoms attached, provides clues to understand that carbon in space is mostly aromatic and partially aliphatic in PAHs. PAH hydrogenation is fundamental to assess the contribution of PAHs to the formation of cosmic H2.
- ItemNon-synchronization of lattice and carrier temperatures in light-emitting diodes([London] : Macmillan Publishers Limited, part of Springer Nature, 2016) Zhang, Jihong; Shih, Tienmo; Lu, Yijun; Merlitz, Holger; Chang, Richard Ru-Gin; Chen, ZhongPulse implementation or switching-off (PISO) of electrical currents has become a common operation in junction-temperature (Tj) measurements for semiconductor devices since 2004. Here we have experimentally discovered a substantial discrepancy between Tj values with and without, PISO (e.g., 36.8 °C versus 76.5 °C above the ambient temperature at 25.0 °C). Our research indicates that methods associated with PISO are flawed due to non-synchronization of lattice temperatures and carrier temperatures in transient states. To scrutinize this discrepancy, we propose a lattice-inertia thermal anchoring mechanism that (1) explains the cause of this discrepancy, (2) helps to develop a remedy to eliminate this discrepancy by identifying three transient phases, (3) has been applied to establishing an original, accurate and noninvasive technique for light-emitting diodes to measure Tj in the absence of PISO. Our finding may pave the foundation for LED communities to further establish reliable junction-temperature measurements based on the identified mechanism.
- ItemPrecise AuxPt1-x Alloy Nanoparticle Array of Tunable Composition for Catalytic Applications([London] : Macmillan Publishers Limited, part of Springer Nature, 2016) Jahn, Sarah; Lechner, Sebastian J.; Freichels, Helene; Möller, Martin; Spatz, Joachim P.A 3-dimensional Block Copolymer Micellar nanoLithography (BCML) process was used to prepare AuxPt1−x alloy nanoparticles (NPs) monodisperse in size and composition, strongly anchored onto SiO2-particles (0.2 wt.% AuxPt1−x/SiO2). The particles possess a face-centered cubic (fcc) crystal structure and their size could be varied from 3–12 nm. We demonstrate the uniformity of the Au/Pt composition by analyzing individual NPs by energy-dispersive X-ray spectroscopy. The strongly bound AuxPt1−x NPs catalyzed the oxidation of CO with high activity. Thermal ageing experiments in pure CO2 as well as in ambient atmosphere demonstrated stability of the size distribution for times as long as 22 h.
- ItemLocalized crystallization in shear bands of a metallic glass([London] : Macmillan Publishers Limited, part of Springer Nature, 2016) Yan, Zhijie; Song, Kaikai; Hu, Yong; Dai, Fuping; Chu, Zhibing; Eckert, JürgenStress-induced viscous flow is the characteristic of atomic movements during plastic deformation of metallic glasses in the absence of substantial temperature increase, which suggests that stress state plays an important role in mechanically induced crystallization in a metallic glass. However, it is poorly understood. Here, we report on the stress-induced localized crystallization in individual shear bands of Zr60Al15Ni25 metallic glass subjected to cold rolling. We find that crystallization in individual shear bands preferentially occurs in the regions neighboring the amorphous matrix, where the materials are subjected to compressive stresses demonstrated by our finite element simulations. Our results provide direct evidence that the mechanically induced crystallization kinetics is closely related with the stress state. The crystallization kinetics under compressive and tensile stresses are interpreted within the frameworks of potential energy landscape and classical nucleation theory, which reduces the role of stress state in mechanically induced crystallization in a metallic glass.
- ItemOn the Dynamical Regimes of Pattern-Accelerated Electroconvection([London] : Macmillan Publishers Limited, part of Springer Nature, 2016) Davidson, Scott M.; Wessling, Matthias; Mani, AliRecent research has established that electroconvection can enhance ion transport at polarized surfaces such as membranes and electrodes where it would otherwise be limited by diffusion. The onset of such overlimiting transport can be influenced by the surface topology of the ion selective membranes as well as inhomogeneities in their electrochemical properties. However, there is little knowledge regarding the mechanisms through which these surface variations promote transport. We use high-resolution direct numerical simulations to develop a comprehensive analysis of electroconvective flows generated by geometric patterns of impermeable stripes and investigate their potential to regularize electrokinetic instabilities. Counterintuitively, we find that reducing the permeable area of an ion exchange membrane, with appropriate patterning, increases the overall ion transport rate by up to 80%. In addition, we present analysis of nonpatterned membranes and find a novel regime of electroconvection where a multivalued current is possible due to the coexistence of multiple convective states.
- ItemSurface effects of vapour-liquid-solid driven Bi surface droplets formed during molecular-beam-epitaxy of GaAsBi([London] : Macmillan Publishers Limited, part of Springer Nature, 2016) Steele, J.A.; Lewis, R.A.; Horvat, J.; Nancarrow, M.J.B.; Henini, M.; Fan, D.; Mazur, Y.I.; Schmidbauer, M.; Ware, M.E.; Yu, S.-Q.; Salamo, G.J.Herein we investigate a (001)-oriented GaAs1−xBix/GaAs structure possessing Bi surface droplets capable of catalysing the formation of nanostructures during Bi-rich growth, through the vapour-liquid-solid mechanism. Specifically, self-aligned “nanotracks” are found to exist trailing the Bi droplets on the sample surface. Through cross-sectional high-resolution transmission electron microscopy the nanotracks are revealed to in fact be elevated above surface by the formation of a subsurface planar nanowire, a structure initiated mid-way through the molecular-beam-epitaxy growth and embedded into the epilayer, via epitaxial overgrowth. Electron microscopy studies also yield the morphological, structural and chemical properties of the nanostructures. Through a combination of Bi determination methods the compositional profile of the film is shown to be graded and inhomogeneous. Furthermore, the coherent and pure zincblende phase property of the film is detailed. Optical characterisation of features on the sample surface is carried out using polarised micro-Raman and micro-photoluminescence spectroscopies. The important light producing properties of the surface nanostructures are investigated through pump intensity-dependent micro-PL measurements, whereby relatively large local inhomogeneities are revealed to exist on the epitaxial surface for important optical parameters. We conclude that such surface effects must be considered when designing and fabricating optical devices based on GaAsBi alloys.
- ItemDistinguishing autocrine and paracrine signals in hematopoietic stem cell culture using a biofunctional microcavity platform([London] : Macmillan Publishers Limited, part of Springer Nature, 2016) Müller, Eike; Wang, Weijia; Qiao, Wenlian; Bornhäuser, Martin; Zandstra, Peter W.; Werner, Carsten; Pompe, TiloHomeostasis of hematopoietic stem cells (HSC) in the mammalian bone marrow stem cell niche is regulated by signals of the local microenvironment. Besides juxtacrine, endocrine and metabolic cues, paracrine and autocrine signals are involved in controlling quiescence, proliferation and differentiation of HSC with strong implications on expansion and differentiation ex vivo as well as in vivo transplantation. Towards this aim, a cell culture analysis on a polymer microcavity carrier platform was combined with a partial least square analysis of a mechanistic model of cell proliferation. We could demonstrate the discrimination of specific autocrine and paracrine signals from soluble factors as stimulating and inhibitory effectors in hematopoietic stem and progenitor cell culture. From that we hypothesize autocrine signals to be predominantly involved in maintaining the quiescent state of HSC in single-cell niches and advocate our analysis platform as an unprecedented option for untangling convoluted signaling mechanisms in complex cell systems being it of juxtacrine, paracrine or autocrine origin.
- ItemMagnetic domain wall gratings for magnetization reversal tuning and confined dynamic mode localization([London] : Macmillan Publishers Limited, part of Springer Nature, 2016) Trützschler, Julia; Sentosun, Kadir; Mozooni, Babak; Mattheis, Roland; McCord, JeffreyHigh density magnetic domain wall gratings are imprinted in ferromagnetic-antiferromagnetic thin films by local ion irradiation by which alternating head-to-tail-to-head-to-tail and head-to-head-to-tail-to-tail spatially overlapping domain wall networks are formed. Unique magnetic domain processes result from the interaction of anchored domain walls. Non-linear magnetization response is introduced by the laterally distributed magnetic anisotropy phases. The locally varying magnetic charge distribution gives rise to localized and guided magnetization spin-wave modes directly constrained by the narrow domain wall cores. The exchange coupled multiphase material structure leads to unprecedented static and locally modified dynamic magnetic material properties.
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