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- ItemFormation mechanism for stable hybrid clusters of proteins and nanoparticles(Washington D.C. : American Chemical Society, 2015) Moerz, Sebastian T.; Kraegeloh, Annette; Chanana, Munish; Kraus, TobiasCitrate-stabilized gold nanoparticles (AuNP) agglomerate in the presence of hemoglobin (Hb) at acidic pH. The extent of agglomeration strongly depends on the concentration ratio [Hb]/[AuNP]. Negligible agglomeration occurs at very low and very high [Hb]/[AuNP]. Full agglomeration and precipitation occur at [Hb]/[AuNP] corresponding to an Hb monolayer on the AuNP. Ratios above and below this value lead to the formation of an unexpected phase: stable, microscopic AuNP–Hb agglomerates. We investigated the kinetics of agglomeration with dynamic light scattering and the adsorption kinetics of Hb on planar gold with surface-acoustic wave-phase measurements. Comparing agglomeration and adsorption kinetics leads to an explanation of the complex behavior of this nanoparticle–protein mixture. Agglomeration is initiated either when Hb bridges AuNP or when the electrostatic repulsion between AuNP is neutralized by Hb. It is terminated when Hb has been depleted or when Hb forms multilayers on the agglomerates that stabilize microscopic clusters indefinitely.
- ItemSintering of ultrathin gold nanowires for transparent electronics(Washington D.C. : American Chemical Society, 2015) Maurer, Johannes H.M.; González-GarcÃa, Lola; Reiser, Beate; Kanelidis, Ioannis; Kraus, TobiasUltrathin gold nanowires (AuNWs) with diameters below 2 nm and high aspect ratios are considered to be a promising base material for transparent electrodes. To achieve the conductivity expected for this system, oleylamine must be removed. Herein we present the first study on the conductivity, optical transmission, stability, and structure of AuNW networks before and after sintering with different techniques. Freshly prepared layers consisting of densely packed AuNW bundles were insulating and unstable, decomposing into gold spheres after a few days. Plasma treatments increased the conductivity and stability, coarsened the structure, and left the optical transmission virtually unchanged. Optimal conditions reduced sheet resistances to 50 Ω/sq.
- ItemAgeing of alkylthiol-stabilized gold nanoparticles(Hoboken, NJ : Wiley, 2015) Lacava, Johann; Weber, Anika; Kraus, TobiasThe ageing of spherical gold nanoparticles having 6-nm-diameter cores and a ligand shell of dodecanethiol is investigated under different storage conditions. Losses caused by agglomeration and changes in optical particle properties are quantified. Changes in colloidal stability are probed by analytical centrifugation in a polar solvent mixture. Chemical changes are detected by elementary analysis of particles and solvent. Fractionation occurs under all storage conditions. Ageing is not uniform but broadens the property distributions of the particles. Small-number statistics in the ligand shell density and the morphological heterogeneity of particles are possible explanations. Washing steps exacerbate ageing, a process that could not be fully reversed by excess ligands. Dry storage is not preferable to storage in solvent. Storage under inert argon atmosphere reduces losses more than all other conditions but could not prevent it entirely.
- ItemRobust, ultrasmall organosilica nanoparticles without silica shells(Heidelberg : Springer, 2014) Murray, Eoin; Born, Philip; Weber, Anika; Kraus, TobiasTraditionally, organosilica nanoparticles have been prepared inside micelles with an external silica shell for mechanical support. Here, we compare these hybrid core–shell particles with organosilica particles that are robust enough to be produced both inside micelles and alone in a sol–gel process. These particles form from octadecyltrimethoxy silane as silica source either in microemulsions, resulting in water-dispersible particles with a hydrophobic core, or precipitate from an aqueous mixture to form particles with both hydrophobic core and surface. We examine size and morphology of the particles by dynamic light scattering and transmission electron microscopy and show that the particles consist of Si–O–Si networks pervaded by alkyl chains using nuclear magnetic resonance, infrared spectroscopy, and thermogravimetric analysis.
- 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.
- ItemMechanism and determinants of nanoparticle penetration through human skin(Cambridge : Royal Society of Chemistry, 2011) Kraus, Tobias; Labouta, Hagar I.; El-Khordagui, Labiba K.; Schneider, MarcThe ability of nanoparticles to penetrate the stratum corneum was the focus of several studies. Yet, there are controversial issues available for particle penetration due to different experimental setups. Meanwhile, there is little known about the mechanism and determinants of their penetration. In this paper the penetration of four model gold nanoparticles of diameter 6 and 15 nm, differing in surface polarity and the nature of the vehicle, through human skin was studied using multiphoton microscopy. This is in an attempt to profoundly investigate the parameters governing particle penetration through human skin. Our results imply that nanoparticles at this size range permeate the stratum corneum in a similar manner to drug molecules, mainly through the intercellular pathways. However, due to their particulate nature, permeation is also dependent on the complex microstructure of the stratum corneum with its tortuous aqueous and lipidic channels, as shown from our experiments performed using skin of different grades of barrier integrity. The vehicle (toluene-versus-water) had a minimal effect on skin penetration of gold nanoparticles. Other considerations in setting up a penetration experiment for nanoparticles were also studied. The results obtained are important for designing a new transdermal carrier and for a basic understanding of skin–nanoparticle interaction.
- 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.
- ItemX-ray imaging with scintillator-sensitized hybrid organic photodetectors(London : Nature Publishing Group, 2015) Büchele, Patric; Richter, Moses; Tedde, Sandro F.; Matt, Gebhard J.; Ankah, Genesis N.; Fischer, Rene; Biele, Markus; Metzger, Wilhelm; Lilliu, Samuele; Bikondoa, Oier; Macdonald, J. Emyr; Brabec, Christoph J.; Kraus, Tobias; Lemmer, Uli; Schmidt, OliverMedical X-ray imaging requires cost-effective and high-resolution flat-panel detectors for the energy range between 20 and 120 keV. Solution-processed photodetectors provide the opportunity to fabricate detectors with a large active area at low cost. Here, we present a disruptive approach that improves the resolution of such detectors by incorporating terbium-doped gadolinium oxysulfide scintillator particles into an organic photodetector matrix. The X-ray induced light emission from the scintillators is absorbed within hundreds of nanometres, which is negligible compared with the pixel size. Hence, optical crosstalk, a limiting factor in the resolution of scintillator-based X-ray detectors, is minimized. The concept is validated with a 256 × 256 pixel detector with a resolution of 4.75 lp mm−1 at a MTF = 0.2, significantly better than previous stacked scintillator-based flat-panel detectors. We achieved a resolution that proves the feasibility of solution-based detectors in medical applications. Time-resolved electrical characterization showed enhanced charge carrier mobility with increased scintillator filling, which is explained by morphological changes.
- ItemOrganosilicate nanoparticles - a familiar material in new shape(Saarbrücken : Leibniz-Institut für Neue Materialien, 2010) Murray, Eoin; Kraus, Tobias[no abstract available]
- ItemThe scale-up of material microstructuring: a perspective(Saarbrücken : Leibniz-Institut für Neue Materialien, 2009) Kraus, Tobias[no abstract available]