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Ulrich Jonas

Publications and source records attributed to Ulrich Jonas.

10 recordsLinked to original sources

Preparation of multilayered trimodal colloid crystals and binary inverse opals.

We report for the first time the preparation of multilayered trimodal colloid crystals (tCC) and their corresponding binary inverse opals (bIO), which present complex hierarchical structures that may have significant potential in photonics, phononics, separations, and catalysis, among others. A trimodal colloidal mixture of 465 nm polystyrene (PS), 84 nm poly(methyl methacrylate) (PMMA), and 6 nm silica particles in suspension was transferred onto a glass substrate and self-assembled into highly ordered trimodal crystal structures during vertical lifting deposition. Pyrolysis of the organic particles in the tCC resulted in silica bIO with interconnected meso- and macropores. Vis-NIR spectra of all structures were analyzed to reveal the internal architecture with each PS sphere correlating to 21-23 PMMA particles (a LI21-23 stoichiometry), which corresponded well with computer models.

Journal Article↗

Observation and tuning of hypersonic bandgaps in colloidal crystals.

Composite materials with periodic variations of density and/or sound velocities, so-called phononic crystals, can exhibit bandgaps where propagation of acoustic waves is forbidden. Phononic crystals are the elastic analogue of the well-established photonic crystals and show potential for manipulating the flow of elastic energy. So far, the experimental realization of phononic crystals has been restricted to macroscopic systems with sonic or ultrasonic bandgaps in the sub-MHz frequency range. In this work, using high-resolution Brillouin spectroscopy we report the first observation of a hypersonic bandgap in face-centred-cubic colloidal crystals formed by self-assembly of polystyrene nanoparticles with subsequent fluid infiltration. Depending on the particle size and the sound velocity in the infiltrated fluid, the frequency and the width of the gap can be tuned. Promising technological applications of hypersonic crystals, ranging from tunable filters and heat management to acousto-optical devices, are anticipated.

Journal Article↗

Parameters influencing the templated growth of colloidal crystals on chemically patterned surfaces.

The influence of various experimental parameters on the vertical deposition and structure formation of colloidal crystals on chemically patterned surfaces, with hydrophilic and hydrophobic areas, was investigated. The pattern dimensions range from about 4 to 400 microm, which is much larger than the individual particle size (255 nm), to control the microscopic crystal shape rather than influencing the crystal lattice geometry (as achieved in colloidal epitaxy). The deposition resolution and selectivity were tested by varying the particle concentration in the suspension, the substrate withdrawing speed, pattern size and orientation, and wetting contrast between the hydrophilic and hydrophobic regions. The evolution of colloidal crystal thickness with respect to the pattern dimensions and deposition parameters was further studied. Our results show that the pattern size has a rather strong influence on the deposited number of colloid layers and on the crystal quality. Better results are obtained when the lines of a stripe pattern are oriented parallel to the withdrawing direction rather than perpendicular. The deposition resolution (defined as the minimum feature size on which particles can be deposited) depends on the wetting contrast and increases with lower average hydrophobicity of the substrate.

Colloids↗

The role of intermolecular and molecule-substrate interactions in the stability of alkanethiol nonsaturated phases on Au(111).

The structure and stability of alkanethiols self-assembled on Au(111) have been studied as a function of the molecular chain length by means of atomic force microscopy (AFM) and grazing incidence X-ray diffraction (GIXD). Below saturation, phases consisting of molecules with different tilt angles and periodicities are formed. Differences in the mechanical stability of these phases are revealed by AFM experiments and discussed in terms of the competition between intermolecular and molecule-substrate interactions as a function of chain length. For long molecules, intermolecular interactions play a dominant role which stabilizes the formation of closed packed 30 degrees tilted ( radical 3x radical 3)R30 degrees structures. For short molecules, the van der Waals interaction with the gold substrate favors the formation of a 50 degrees tilted phase in which the molecules are arranged in a rectangular configuration.

Journal Article↗

Synthesis and pH-selective adsorption of latex particles onto photolithographically patterned silane layers.

Surface structures of charged latex particles on patterned surface layers were obtained by a colloidal self-assembly process. The laterally patterned silane layers were prepared on silica surfaces by vapor phase and solution deposition of silanes in combination with photolithography. The monodisperse latex particles used in the self-assembly experiments were synthesized by emulsion polymerization to yield poly-n-butylmethacrylate spheres (217 nm diameter) and poly-n-butylacrylate microgels (155 nm). Both particle types possessed a high surface concentration of free carboxylic acid groups as quantified by polyelectrolyte titration under shear flow. Depending on the pH, the particles assembled onto the hydrophobic surface regions (pH 9) or onto the hydrophilic regions (pH 5). Highest selectivity and pattern quality was obtained with permanently positively charged silane layers (quaternary ammonium salts) onto which the negatively charged colloid particles adhered strongly by Coulomb interaction.

Journal Article↗

Colloidal assemblies on patterned silane layers.

The site-selective assembly of colloidal polymer particles onto laterally patterned silane layers was studied as a model system for the object assembly process at mesoscale dimensions. The structured silane monolayers on silicon oxide substrates were fabricated by a combination of liquid- and gas-phase deposition of different trialkoxysilanes with a photolithographic patterning technique. By using this method various types of surface functionalizations such as regions with amino functions next to areas of the bare silica surface or positively charged regions of a quaternary ammonium silane surrounded by a hydrophobic octadecylsilane film could be obtained. Furthermore, a triethoxysilane with a photoprotected amino group was synthesized, which allowed direct photopatterning after monolayer preparation, leading to free NH(2) groups at the irradiated regions. The different silane monolayer patterns were used to study the surface assembly behavior of carboxylated methacrylate particles by optical and scanning electron microscopy. In dependence of the assembly conditions (different surface functionalizations, pH, and drying conditions), a selective preference of the particles for a specific surface type versus others was found. Site-specific colloid adsorption could be observed also on the photosensitive silane layers after local deprotection with light. From the photosensitive silane and positively charged ammonium silane, molecularly mixed monolayers were prepared, which allowed particle adsorption and photoactivation within the same monolayer as shown by fluorescence labeling.

Carboxylic Acids↗

Direct conversion of EPR dipolar time evolution data to distance distributions.

Shallow electron spin echo envelope modulations due to dipole-dipole couplings between electron spins provide information on the radial distribution function of the spins in disordered systems while angular correlations between spin pairs are negligible. Under these conditions and in the absence of orientational selection, the dipolar time evolution data can be quantitatively simulated for arbitrary radial distribution functions by shell factorization, i.e., by performing the orientational average separately for thin spherical shells and multiplying the signals of all the shells. For distances below 5 nm, a linear superposition of the signals of the shells is sufficient. The dipolar time evolution data can be separated into this linear contribution and a nonlinear background. The linear contribution can then be converted directly to a radial distribution function. For a series of shape-persistent and flexible biradicals with end-to-end distances between 2 and 5 nm, shell factorization and direct conversion of the data are in good agreement with each other and with force-field computations of the end-to-end distances. The neglect of orientation selection does not cause significant distortions of the determined distance distributions.

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