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Item type:Publication, Access status: with files , Self-detachment and subsurface densification of dealloyed nanoporoust thin films(American Chemical Society (ACS), 2022-08-24); ; ; ; Experiment shows thin films of dealloyed nanoporous gold (NPG) spontaneously detaching from massive gold base layers. NPG can also densify near its external surface. This is naturally reproduced by kinetic Monte Carlo (KMC) simulation of dealloying and coarsening and so appears generic for nanoscale network materials evolving by surface diffusion. Near the porous layer's external surface and near its interface with the base layer, gradients in the depth-profile of a laterally averaged mean surface curvature provide driving forces for diffusion and cause divergences of the net fluxes of matter, leading to accretion/densification or to erosion/disconnection. As a toy model, the morphology evolution of substrate-supported nanopillars by surface diffusion illustrates and confirms our considerations. Contrary to cylindrical nanowires, the ligaments in nanoporous materials exhibit pre-existing gradients in the mean curvature. The Plateau-Rayleigh long-wavelength stability criterion is then not applicable and the disconnection accelerated.Publicationtype: Journal ArticleScopus© Citations 9 55 161 - Some of the metrics are blocked by yourconsent settings
Item type:Publication, Access status: with files , Spin‐ and Stress‐Depending Electrical Transport in Nanoparticle Supercrystals: Sensing Elastic Properties of Organic Tunnel Barriers via Tunneling Magnetoresistance(Wiley-VCH, 2022-05-26); ; ; ; Abstract The spin‐dependent electrical transport in rigid inorganic‐inorganic layered systems is extensively applied for the detection of magnetic fields in data storage. In this work, spin‐dependent electrical transport in flexible organic‐inorganic supercrystals based on superparamagnetic iron oxide nanoparticles is investigated. These nanoparticles are stabilized by oleic acid ligands, which in turn are serving as tunneling barriers between individual magnetic nanoparticles. The resulting tunneling magnetoresistance (TMR) is tunable due to the elastic properties of these organic barriers. Applying external mechanical stress on this composite material will change the average distance between adjacent nanoparticles and will hence determine the resulting TMR‐effect amplitude. Thus, measured stress‐induced changes in the barrier thickness at sub‐nanometer scale allow for determining the mechanical properties of organic barrier molecules in the confined space between the particles. These results provide the foundation for a new type of mechanical sensor.Publicationtype: Journal ArticleScopus© Citations 3 89 163 - Some of the metrics are blocked by yourconsent settings
Item type:Publication, Access status: with files , Constitutive and fracture behavior of ultra-strong supercrystalline nanocomposites(American Institute of Physics (AIP), 2021-09-09); ; ; ; Supercrystalline nanocomposites are a new class of hybrid and nanostructured materials that can reach exceptional mechanical strength and can be fabricated at low temperatures. Hierarchically arranged, they bridge the gap from the nano- to the macro-scale. Even though their mechanical properties are starting to be characterized, their constitutive behavior is still largely unexplored. Here, the mechanical behavior of supercrystalline nanocomposites of iron oxide nanoparticles, surface-functionalized with oleic acid and oleyl phosphate ligands, is investigated in both bending and compression, with loading-unloading tests. A new bar geometry is implemented to better detect deformation prior to unstable crack propagation, and notched bending bars are tested to evaluate fracture toughness. Micro-mechanical tests result in the values of strength and elastic modulus that are extremely high for supercrystals, reaching record-high numbers in the oleic acid-based nanocomposites, which also show a significant tension-compression asymmetry. The constitutive behavior of both materials is predominantly linear elastic, with some more marked nonlinearities arising in the oleyl phosphate-based nanocomposites. The fracture toughness of both types of nanocomposites, ∼0.3 MPa√m, suggests that extrinsic toughening, associated with both material composition and nanostructure, plays an important role. Fractographic observations reveal analogies with shear and cleavage in atomic crystals. The influence of material composition, nanostructure, and processing method on the mechanical behavior of the nanocomposites is analyzed.Publicationtype: Journal ArticleScopus© Citations 8 106 269 - Some of the metrics are blocked by yourconsent settings
Item type:Publication, Access status: with files , Deformation behavior of cross-linked supercrystalline nanocomposites: an in situ SAXS/WAXS study during uniaxial compression(American Chemical Society (ACS), 2021-03-22); ; ; ; With the ever-expanding functional applications of supercrystalline nanocomposites (a relatively new category of materials consisting of organically functionalized nanoparticles arranged into periodic structures), it becomes necessary to ensure their structural stability and understand their deformation and failure mechanisms. Inducing the cross-linking of the functionalizing organic ligands, for instance, leads to a remarkable enhancement of the nanocomposites' mechanical properties. It is however still unknown how the cross-linked organic phase redistributes applied loads, how the supercrystalline lattice accommodates the imposed deformations, and thus in general what phenomena govern the overall material's mechanical response. This work elucidates these aspects for cross-linked supercrystalline nanocomposites through an in situ small- and wide-angle X-ray scattering study combined with uniaxial pressing. Because of this loading condition, it emerges that the cross-linked ligands effectively carry and distribute loads homogeneously throughout the nanocomposites, while the superlattice deforms via rotation, slip, and local defects generation.Publicationtype: Journal ArticleScopus© Citations 12 181 313 - Some of the metrics are blocked by yourconsent settings
Item type:Publication, Access status: with files , Influence of the experimental set-up and voltage ramp on the dielectric breakdown strength and breakdown site in borosilicate glass(2021-02-02); The dielectric breakdown strength of borosilicate glass and alumina was measured as a function of the voltage ramp rate on different material thicknesses and with different electrode configurations. While this is not a completely new approach, with our work we want to highlight the importance of appropriate measurement set-up and contribute to a better understanding and analysis of dielectric breakdown. The measurement of breakdown tests is generally anything but trivial and the comparison of breakdown results for different set-ups is difficult, especially because not all scientific articles go into detail on the measurement method and all the important parameters, which can influence the breakdown event. For the results shown in this work we mainly used glass as a suitable model material and two different electrode setups at eleven different voltage ramps in the range of 5 V/s to 10,000 V/s. We found that there is a clear dependence of the dielectric breakdown strength on the voltage ramp and the electrode configuration as well as it should be distinguished between breakdowns which initiated at electrode edge and those initiated within the electrode area. There is almost no scatter for breakdown strengths which were initiated inside a silver paste electrode in comparison to breakdown strength from the electrode edges.Publicationtype: Journal ArticleScopus© Citations 4 179 856 - Some of the metrics are blocked by yourconsent settings
Item type:Publication, Access status: with files , Defects and plasticity in ultrastrong supercrystalline nanocomposites(2021-01-06); ; ; ; Supercrystalline nanocomposites are nanoarchitected materials with a growing range of applications but unexplored in their structural behavior. They typically consist of organically functionalized inorganic nanoparticles arranged into periodic structures analogous to crystalline lattices, including superlattice imperfections induced by processing or mechanical loading. Although featuring a variety of promising functional properties, their lack of mechanical robustness and unknown deformation mechanisms hamper their implementation into devices. We show that supercrystalline materials react to indentation with the same deformation patterns encountered in single crystals. Supercrystals accommodate plastic deformation in the form of pile-ups, dislocations, and slip bands. These phenomena occur, at least partially, also after cross-linking of the organic ligands, which leads to a multifold strengthening of the nanocomposites. The classic shear theories of crystalline materials are found to describe well the behavior of supercrystalline nanocomposites, which result to feature an elastoplastic behavior, accompanied by compaction.Publicationtype: Journal ArticleScopus© Citations 15 239 217 - Some of the metrics are blocked by yourconsent settings
Item type:Publication, Access status: with files , Controlling the large-scale fabrication of supraparticlesControlling the nanoscale interactions of colloidal building blocks is a key step for the transition from single nanoparticles to tailor-made, architected morphologies and their further integration into functional materials. Solvent evaporation-induced self-assembly within emulsion droplets emerges as a fast, versatile, and low-cost approach to obtain spherical, complex structures, such as supraparticles. Nevertheless, some process-structure relationships able to describe the effects of emulsion conditions on the synthesis outcomes still remain to be understood. Here, we explore the effect of different physicochemical parameters of emulsion-templated self-assembly (ETSA) on supraparticles' formation. Supraparticle size, size dispersity, microporosity, and sample homogeneity are rationalized based on the used surfactant formulation, stabilization mechanism, and viscosity of the emulsion. We further demonstrate the significance of the parameters found by optimizing a transferable, large-scale (gram-size) ETSA setup for the controlled synthesis of spherical supraparticles in a range of defined sizes (from 0.1-10 μm). Ultimately, our results provide new key synthetic parameters able to control the process, promoting the development of supraparticle-based, functional nanomaterials for a wide range of applications.Publicationtype: Journal ArticleScopus© Citations 13 199 392 - Some of the metrics are blocked by yourconsent settings
Item type:Publication, Access status: with files , Mapping the mechanical properties of hierarchical supercrystalline ceramic-organic nanocomposites(Multidisciplinary Digital Publishing Institute (MDPI), 2020-10-19); ; ; ; Multiscale ceramic-organic supercrystalline nanocomposites with two levels of hierarchy have been developed via self-assembly with tailored content of the organic phase. These nanocomposites consist of organically functionalized ceramic nanoparticles forming supercrystalline micron-sized grains, which are in turn embedded in an organic-rich matrix. By applying an additional heat treatment step at mild temperatures (250–350 °C), the mechanical properties of the hierarchical nanocomposites are here enhanced. The heat treatment leads to partial removal and crosslinking of the organic phase, minimizing the volume occupied by the nanocomposites’ soft phase and triggering the formation of covalent bonds through the organic ligands interfacing the ceramic nanoparticles. Elastic modulus and hardness up to 45 and 2.5 GPa are attained, while the hierarchical microstructure is preserved. The presence of an organic phase between the supercrystalline grains provides a toughening effect, by curbing indentation-induced cracks. A mapping of the nanocomposites’ mechanical properties reveals the presence of multiple microstructural features and how they evolve with heat treatment temperature. A comparison with non-hierarchical, homogeneous supercrystalline nanocomposites with lower organic content confirms how the hierarchy-inducing organic excess results in toughening, while maintaining the beneficial effects of crosslinking on the materials’ stiffness and hardness.Publicationtype: Journal ArticleScopus© Citations 10 290 329 - Some of the metrics are blocked by yourconsent settings
Item type:Publication, Access status: with files , Ultra-thin and ultra-strong organic interphase in nanocomposites with supercrystalline particle arrangement : mechanical behavior identification via multiscale numerical modeling(Elsevier, 2020-09-29); ; ; ; © 2020 The Authors. A key challenge in the development of inorganic-organic nanocomposites is the mechanical behavior identification of the organic phase. For supercrystalline materials, in which the organic phase ranges down to sub-nm areas, the identification of the organic materials' mechanical properties is however experimentally inaccessible. The supercrystalline nanocomposites investigated here are 3D superlattices of self-assembled iron oxide nanoparticles, surface-functionalized with crosslinked oleic acid ligands. They exhibit the highest reported values of Young's modulus, nanohardness and strength for inorganic-organic nanocomposites. A multiscale numerical modeling approach is developed to identify these properties using supercrystalline representative volume elements, in which the nanoparticles are arranged in a face-centered cubic superlattice and the organic phase is modeled as a thin layer interfacing each particle. A Drucker-Prager-type elastoplastic constitutive law with perfectly plastic yielding is identified as being able to describe the supercrystals' response in nanoindentation accurately. As the nanoparticles behave in a purely elastic manner with very high stiffness, the underlying constitutive law of the organic phase is also identified to be Drucker-Prager-type elastoplastic, with a Young's modulus of 13 GPa and a uniaxial tensile yield stress of 900 MPa, remarkably high values for an organic material, and matching well with experimental and DFT-based estimations. Furthermore, a sensitivity study indicates that small configurational changes within the supercrystalline lattice do not significantly alter the overall stiffness behavior. Multiscale numerical modeling is thus proven to be able to identify the nanomechanical properties of supercrystals, and can ultimately be used to tailor these materials' mechanical behavior starting from superlattice considerations.Publicationtype: Journal ArticleScopus© Citations 12 268 361 - Some of the metrics are blocked by yourconsent settings
Item type:Publication, Access status: with files , Strong macroscale supercrystalline structures by 3D printing combined with self-assembly of ceramic functionalized nanoparticles(Wiley-VCH, 2020-04-29); ; ; ; To translate the exceptional properties of colloidal nanoparticles (NPs) to macroscale geometries, assembly techniques must bridge a 106-fold range of length. Moreover, for successfully attaining a final mechanically robust nanocomposite macroscale material, some of the intrinsic NPs’ properties have to be maintained while minimizing the density of strength-limiting defects. However, the assembly of nanoscale building blocks into macroscopic dimensions, and their effective macroscale properties, are inherently affected by the precision of the conditions required for assembly and emergent flaws including point defects, dislocations, grain boundaries, and cracks. Herein, a direct-write self-assembly technique is used to construct free-standing, millimeter-scale columns comprising spherical iron oxide NPs (15 nm diameter) surface functionalized with oleic acid (OA), which self-assemble into face-centered cubic (FCC) supercrystals in minutes during the direct-writing process. The subsequent crosslinking of OA molecules results in nanocomposites with a maximum strength of 110 MPa and elastic modulus up to 58 GPa. These mechanical properties are interpreted according to the flaw size distribution and are as high as newly engineered platelet-based nanocomposites. The findings indicate a broad potential to create mechanically robust, multifunctional 3D structures by combining additive manufacturing with colloidal assembly.Publicationtype: Journal ArticleScopus© Citations 17 304 287