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- ItemPrograming stimuli-responsiveness of gelatin with electron beams: Basic effects and development of a hydration-controlled biocompatible demonstrator(London : Nature Publishing Group, 2017) Riedel, Stefanie; Heyart, Benedikt; Apel, Katharina S.; Mayr, Stefan G.Biomimetic materials with programmable stimuli responsiveness constitute a highly attractive material class for building bioactuators, sensors and active control elements in future biomedical applications. With this background, we demonstrate how energetic electron beams can be utilized to construct tailored stimuli responsive actuators for biomedical applications. Composed of collagen-derived gelatin, they reveal a mechanical response to hydration and changes in pH-value and ion concentration, while maintaining their excellent biocompatibility and biodegradability. While this is explicitly demonstrated by systematic characterizing an electron-beam synthesized gelatin-based actuator of cantilever geometry, the underlying materials processes are also discussed, based on the fundamental physical and chemical principles. When applied within classical electron beam lithography systems, these findings pave the way for a novel class of highly versatile integrated bioactuators from micro-to macroscales.
- ItemDC conductivity and Seebeck coefficient of nonstoichiometric MgCuZn ferrites(Warsaw : De Gruyter Open, 2017-2-8) Madhuri, W.; Kiran, S. Roopas; Reddy, M. Penchal; Reddy, N. Ramamanohar; Kumar, K.V. SivaNonstoichiometric series of Mg0.5-xCuxZn0.5Fe1.9O4-δ where x = 0.0, 0.1, 0.15, 0.2 and 0.25 has been synthesized by conventional solid state reaction route. The single phase spinel structure of the double sintered ferrites was confirmed by X-ray diffraction patterns (XRD). The ferrite series was studied in terms of DC electrical conductivity and thermoelectric power in the temperature ranging from room temperature to 300 °C and 400 °C, respectively. It was observed that DC electrical conductivity and Seebeck coefficient α decreased with the increase in x. DC electrical conductivity was found to decrease by about 4 orders. All the compositions showed a negative Seebeck coefficient exhibiting n-type semiconducting nature. From the above experimental results, activation energy and mobility of all the samples were estimated. Small polaron hopping conduction mechanism was suggested for the series of ferrites. Owing to their low conductivity the nonstoichiometric MgCuZn ferrites are the best materials for transformer core and high definition television deflection yokes. © 2017 Wroclaw University of Science and Technology.
- ItemNanometer-thick lateral polyelectrolyte micropatterns induce macrosopic electro-osmotic chaotic fluid instabilities([London] : Macmillan Publishers Limited, part of Springer Nature, 2014) Wessling, M.; Morcillo, L. Garrigós; Abdu, S.Electro-convective vortices in ion concentration polarization under shear flow have been of practical relevance for desalination processes using electrodialysis. The phenomenon has been scientifically disregarded for decades, but is recently embraced by a growing fluid dynamics community due its complex superposition of multi-scale gradients in electrochemical potential and space charge interacting with emerging complex fluid momentum gradients. While the visualization, quantification and fundamental understanding of the often-chaotic fluid dynamics is evolving rapidly due to sophisticated simulations and experimentation, little is known whether these instabilities can be induced and affected by chemical topological heterogeneity in surface properties. In this letter, we report that polyelectrolyte layers applied as micropatterns on ion exchange membranes induce and facilitate the electro-osmotic fluid instabilities. The findings stimulate a variety of fundamental questions comparable to the complexity of today's turbulence research.
- ItemMulti-shell hollow nanogels with responsive shell permeability([London] : Macmillan Publishers Limited, part of Springer Nature, 2016) Schmid, Andreas J.; Dubbert, Janine; Rudov, Andrey A.; Pedersen, Jan Skov; Lindner, Peter; Karg, Matthias; Potemkin, Igor I.; Richtering, WalterWe report on hollow shell-shell nanogels with two polymer shells that have different volume phase transition temperatures. By means of small angle neutron scattering (SANS) employing contrast variation and molecular dynamics (MD) simulations we show that hollow shell-shell nanocontainers are ideal systems for controlled drug delivery: The temperature responsive swelling of the inner shell controls the uptake and release, while the thermoresponsive swelling of the outer shell controls the size of the void and the colloidal stability. At temperatures between 32 °C < T < 42 °C, the hollow nanocontainers provide a significant void, which is even larger than the initial core size of the template and they possess a high colloidal stability due to the steric stabilization of the swollen outer shell. Computer simulations showed, that temperature induced switching of the permeability of the inner shell allows for the encapsulation in and release of molecules from the cavity.
- ItemSelf-Regenerating Soft Biophotovoltaic Devices(Washington, DC : ACS Publications, 2018) Qiu, Xinkai; Castañeda Ocampo, Olga; de Vries, Hendrik W.; van Putten, Maikel; Loznik, Mark; Herrmann, Andreas; Chiechi, Ryan C.This paper describes the fabrication of soft, stretchable biophotovoltaic devices that generate photocurrent from photosystem I (PSI) complexes that are self-assembled onto Au electrodes with a preferred orientation. Charge is collected by the direct injection of electrons into the Au electrode and the transport of holes through a redox couple to liquid eutectic gallium-indium (EGaIn) electrodes that are confined to microfluidic pseudochannels by arrays of posts. The pseudochannels are defined in a single fabrication step that leverages the non-Newtonian rheology of EGaIn. This strategy is extended to the fabrication of reticulated electrodes that are inherently stretchable. A simple shadow evaporation technique is used to increase the surface area of the Au electrodes by a factor of approximately 106 compared to planar electrodes. The power conversion efficiency of the biophotovoltaic devices decreases over time, presumably as the PSI complexes denature and/or detach from the Au electrodes. However, by circulating a solution of active PSI complexes the devices self-regenerate by mass action/self-assembly. These devices leverage simple fabrication techniques to produce complex function and prove that photovoltaic devices comprising PSI can retain the ability to regenerate, one of the most important functions of photosynthetic organisms. © 2018 American Chemical Society.
- ItemSeeded Growth Synthesis of Gold Nanotriangles: Size Control, SAXS Analysis, and SERS Performance(Washington, DC : Soc., 2018) Kuttner, Christian; Mayer, Martin; Dulle, Martin; Moscoso, Ana; López-Romero, Juan Manuel; Förster, Stephan; Fery, Andreas; Pérez-Juste, Jorge; Contreras-Cáceres, RafaelWe studied the controlled growth of triangular prismatic Au nanoparticles with different beveled sides for surface-enhanced Raman spectroscopy (SERS) applications. First, in a seedless synthesis using 3-butenoic acid (3BA) and benzyldimethylammonium chloride (BDAC), gold nanotriangles (AuNTs) were synthesized in a mixture with gold nanooctahedra (AuNOCs) and separated by depletion-induced flocculation. Here, the influence of temperature, pH, and reducing agent on the reaction kinetics was initially investigated by UV–vis and correlated to the size and yield of AuNT seeds. In a second step, the AuNT size was increased by seed-mediated overgrowth with Au. We show for the first time that preformed 3BA-synthesized AuNT seeds can be overgrown up to a final edge length of 175 nm and a thickness of 80 nm while maintaining their triangular shape and tip sharpness. The NT morphology, including edge length, thickness, and tip rounding, was precisely characterized in dispersion by small-angle X-ray scattering and in dry state by transmission electron microscopy and field-emission scanning electron microscopy. For sensor purposes, we studied the size-dependent SERS performance of AuNTs yielding analytical enhancement factors between 0.9 × 104 and 5.6 × 104 and nanomolar limit of detection (10–8–10–9 M) for 4-mercaptobenzoic acid and BDAC. These results confirm that the 3BA approach allows the fabrication of AuNTs in a whole range of sizes maintaining the NT morphology. This enables tailoring of localized surface plasmon resonances between 590 and 740 nm, even in the near-infrared window of a biological tissue, for use as colloidal SERS sensing agents or for optoelectronic applications.
- ItemMechanical Robustness of Graphene on Flexible Transparent Substrates(Washington, DC : Soc., 2016) Kang, Moon H.; Prieto López, Lizbeth O.; Chen, Bingan; Teo, Ken; Williams, John A.; Milne, William I.; Cole, Matthew T.This study reports on a facile and widely applicable method of transferring chemical vapor deposited (CVD) graphene uniformly onto optically transparent and mechanically flexible substrates using commercially available, low-cost ultraviolet adhesive (UVA) and hot-press lamination (HPL). We report on the adhesion potential between the graphene and the substrate, and we compare these findings with those of the more commonly used cast polymer handler transfer processes. Graphene transferred with the two proposed methods showed lower surface energy and displayed a higher degree of adhesion (UVA: 4.40 ± 1.09 N/m, HPL: 0.60 ± 0.26 N/m) compared to equivalent CVD-graphene transferred using conventional poly(methyl methacrylate) (PMMA: 0.44 ± 0.06 N/m). The mechanical robustness of the transferred graphene was investigated by measuring the differential resistance as a function of bend angle and repeated bend–relax cycles across a range of bend radii. At a bend angle of 100° and a 2.5 mm bend radius, for both transfer techniques, the normalized resistance of graphene transferred on polyethylene terephthalate (PET) was around 80 times less than that of indium–tin oxide on PET. After 104 bend cycles, the resistance of the transferred graphene on PET using UVA and HPL was found to be, on average, around 25.5 and 8.1% higher than that of PMMA-transferred graphene, indicating that UVA- and HPL-transferred graphene are more strongly adhered compared to PMMA-transferred graphene. The robustness, in terms of maintained electrical performance upon mechanical fatigue, of the transferred graphene was around 60 times improved over ITO/PET upon many thousands of repeated bending stress cycles. On the basis of present production methods, the development of the next-generation of highly conformal, diverse form factor electronics, exploiting the emerging family of two-dimensional materials, necessitates the development of simple, low-cost, and mechanically robust transfer processes; the developed UVA and HPL approaches show significant potential and allow for large-area-compatible, near-room temperature transfer of graphene onto a diverse range of polymeric supports.
- ItemA classical description of subnanometer resolution by atomic features in metallic structures(Cambridge : RSC Publ., 2016) Trautmann, S.; Aizpurua, J.; Götz, I.; Undisz, A.; Dellith, J.; Schneidewind, H.; Rettenmayr, M.; Deckert, V.Recent experiments have evidenced sub-nanometer resolution in plasmonic-enhanced probe spectroscopy. Such a high resolution cannot be simply explained using the commonly considered radii of metallic nanoparticles on plasmonic probes. In this contribution the effects of defects as small as a single atom found on spherical plasmonic particles acting as probing tips are investigated in connection with the spatial resolution provided. The presence of abundant edge and corner sites with atomic scale dimensions in crystalline metallic nanoparticles is evident from transmission electron microscopy (TEM) images. Electrodynamic calculations based on the Finite Element Method (FEM) are implemented to reveal the impact of the presence of such atomic features in probing tips on the lateral spatial resolution and field localization. Our analysis is developed for three different configurations, and under resonant and non-resonant illumination conditions, respectively. Based on this analysis, the limits of field enhancement, lateral resolution and field confinement in plasmon-enhanced spectroscopy and microscopy are inferred, reaching values below 1 nanometer for reasonable atomic sizes.
- ItemPlasmon response evaluation based on image-derived arbitrary nanostructures(Cambridge : RSC Publ., 2018) Trautmann, S.; Richard-Lacroix, M.; Dathe, A.; Schneidewind, H.; Dellith, J.; Fritzsche, W.; Deckert, V.The optical response of realistic 3D plasmonic substrates composed of randomly shaped particles of different size and interparticle distance distributions in addition to nanometer scale surface roughness is intrinsically challenging to simulate due to computational limitations. Here, we present a Finite Element Method (FEM)-based methodology that bridges in-depth theoretical investigations and experimental optical response of plasmonic substrates composed of such silver nanoparticles. Parametrized scanning electron microscopy (SEM) images of surface enhanced Raman spectroscopy (SERS) active substrate and tip-enhanced Raman spectroscopy (TERS) probes are used to simulate the far-and near-field optical response. Far-field calculations are consistent with experimental dark field spectra and charge distribution images reveal for the first time in arbitrary structures the contributions of interparticle hybridized modes such as sub-radiant and super-radiant modes that also locally organize as basic units for Fano resonances. Near-field simulations expose the spatial position-dependent impact of hybridization on field enhancement. Simulations of representative sections of TERS tips are shown to exhibit the same unexpected coupling modes. Near-field simulations suggest that these modes can contribute up to 50% of the amplitude of the plasmon resonance at the tip apex but, interestingly, have a small effect on its frequency in the visible range. The band position is shown to be extremely sensitive to particle nanoscale roughness, highlighting the necessity to preserve detailed information at both the largest and the smallest scales. To the best of our knowledge, no currently available method enables reaching such a detailed description of large scale realistic 3D plasmonic systems.
- 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.