One‐step deposition of nano‐to‐micron‐scalable, high‐quality digital image correlation patterns for high‐strain in‐situ multi‐microscopy testing

Digital image correlation (DIC) is of vital importance in the field of experimental mechanics, yet producing suitable DIC patterns for demanding in-situ (micro)mechanical tests remains challenging, especially for ultrafine patterns, despite the large number of patterning techniques reported in the literature. Therefore, we propose a simple, flexible, one-step technique (only requiring a conventional physical vapour deposition machine) to obtain scalable, high-quality, robust DIC patterns, suitable for a range of microscopic techniques, by deposition of a low-melting temperature solder alloy in the so-called island growth mode, without elevating the substrate temperature. Proof of principle is shown by (near-)room temperature deposition of InSn patterns, yielding highly dense, homogeneous DIC patterns over large areas with a feature size that can be tuned from as small as ~10 nm to ~2 μm and with control over the feature shape and density by changing the deposition parameters. Pattern optimisation, in terms of feature size, density, and contrast, is demonstrated for imaging with atomic force microscopy, scanning electron microscopy, optical profilometry, and optical microscopy. Moreover, the performance of the InSn DIC patterns and their robustness to large deformations is validated in two challenging case studies of in-situ micromechanical testing: (a) self-adaptive isogeometric digital height correlation of optical surface height profiles of a coarse, bimodal InSn pattern providing microscopic 3D deformation fields (illustrated for delamination of Al stretchable interconnects on a PI substrate) and (b) DIC on scanning electron microscopy images of a much finer InSn pattern allowing quantification of high strains near fracture locations (illustrated for rupture of a polycrystalline Fe foil). As such, the high controllability, performance, and scalability of the DIC patterns, created by island growth of a solder alloy, offer a promising step towards more routine DIC-based in-situ micromechanical testing.</p

Manufacturing Free-Standing, Porous Metallic Layers with Dynamic Hydrogen Bubble Templating

The 3D structure (i.e., microstructure) of porous electrodes governs the performance of emerging electrochemical technologies such as fuel cells, electrolysis, and batteries. Sustaining electrochemical reactions and convective-diffusive mass transport at high efficiency is complex and motivates the search for sophisticated microstructures with multimodal pore size distributions and pore size gradients. Here a new synthesis route for porous, metallic layers is presented that combines the characteristics of carbon structures (i.e., pore size, porosity) with the properties of metals (i.e., recyclability, conductivity). Building on the method of dynamic hydrogen bubble templating, a novel approach is engineered to manufacture thin, free-standing layers using an electrochemical flow cell through the introduction of an intermediate layer and optimization of the synthesis parameters. Mechanically stable layers are created with thicknesses ranging from ≈50 to ≈200 µm comprising porous, dendritic structures, arranged to form a vascular network of larger pores with a gradient in radii from ≈5 µm at the bottom and up to ≈36 µm at the top of the material. Using X-ray tomographic data, the morphology is analyzed, and the diffusive transport through the material as a function of liquid filling is simulated and compared to state-of-the-art carbon fiber-based electrodes, showing significantly higher mass transfer properties.</p

Micron-scale experimental-numerical characterization of metal-polymer interface delamination in stretchable electronics interconnects

Understanding the mechanical behavior and failure mechanisms of stretchable electronics is key in developing reliable and long-lasting devices. In this work a micron-scale stretchable system consisting of an aluminum serpentine patterned interconnect adhered to a polyimide substrate is studied. In-situ experiments are performed where the stretchable sample is elongated, while the surface topography is measured using a confocal microscope. From the resulting height profiles the microscopic three-dimensional deformations are extracted using an adaptive isogeometric digital height correlation algorithm. The displacement information is compared to realistic numerical simulations, in which the interface behavior is described by cohesive zone elements. It is concluded that despite fitting the traction separation law parameters, the model fails to correctly capture the distinct out-of-plane buckling (with magnitude of a few micron) of the interconnect. The model is updated with residual stresses resulting from processing and crystal plasticity induced behavior (decreased yield strength) in the aluminum layer, but both measures are not resulting in the experimentally observed deformations. Finally, mixed-mode cohesive zones are implemented, in which the properties are different in the shear and normal direction. After fitting the corresponding parameters to the experimental data, the model shows realistic in-plane and out-of-plane deformations. Also a predictive simulation for a different geometry results in the correct experimentally measured behavior. It is concluded that the aluminum-polyimide interface mode-angle dependency explains the observed microscopic failure mode of local delamination and buckle formation.</p

Micro- and Nanoscale Heterogeneities in Zeolite Beta as measured by Atom Probe Tomography and Confocal Fluorescence Microscopy

Micro- and nanoscale information on the activating and deactivating coking behaviour of zeolite catalyst materials increases our current understanding of many industrially applied processes, such as the methanol-to-hydrocarbon (MTH) reaction. Atom probe tomography (APT) was used to reveal the link between framework and coke elemental distributions in 3D with sub-nanometre resolution. APT revealed 10-20 nanometre-sized Al-rich regions and short-range ordering (within nanometres) between Al atoms. With confocal fluorescence microscopy, it was found that the morphology of the zeolite crystal as well as the secondary mesoporous structures have a great effect on the microscale coke distribution throughout individual zeolite crystals over time. Additionally, a nanoscale heterogeneous distribution of carbon as residue from the MTH reaction was determined with carbon-rich areas of tens of nanometres within the zeolite crystals. Lastly, a short length-scale affinity between C and Al atoms, as revealed by APT, indicates the formation of carbon-containing molecules next to the acidic sites in the zeolite

Combined engineering of disaccharide transport and phosphorolysis for enhanced ATP yield from sucrose fermentation in Saccharomyces cerevisiae

Anaerobic industrial fermentation processes do not require aeration and intensive mixing and the accompanying cost savings are beneficial for production of chemicals and fuels. However, the free-energy conservation of fermentative pathways is often insufficient for the production and export of the desired compounds and/or for cellular growth and maintenance. To increase free-energy conservation during fermentation of the industrially relevant disaccharide sucrose by Saccharomyces cerevisiae, we first replaced the native yeast α-glucosidases by an intracellular sucrose phosphorylase from Leuconostoc mesenteroides (LmSPase) (Figure 1). Subsequently, we replaced the native proton-coupled sucrose uptake system by a putative sucrose facilitator from Phaseolus vulgaris (PvSUF1). The resulting strains grew anaerobically on sucrose at specific growth rates of 0.09 ± 0.02 h-1 (LmSPase) and 0.06 ± 0.01 h-1 (PvSUF1, LmSPase). Overexpression of the yeast PGM2 gene, which encodes phosphoglucomutase, increased anaerobic growth rates on sucrose of these strains to 0.23 ± 0.01 h-1 and 0.08 ± 0.00 h-1, respectively. Determination of the biomass yield in anaerobic sucrose-limited chemostat cultures was used to assess the free-energy conservation of the engineered strains. Replacement of intracellular hydrolase with a phosphorylase increased the biomass yield on sucrose by 31%. Additional replacement of the native proton-coupled sucrose uptake system by PvSUF1 increased the anaerobic biomass yield by a further 8%, resulting in an overall increase of 41%. By experimentally demonstrating an energetic benefit of the combined engineering of disaccharide uptake and cleavage, this study represents a first step towards anaerobic production of compounds whose metabolic pathways currently do not conserve sufficient free-energy. Please click Additional Files below to see the full abstract

Molecular Accessibility and Diffusion of Resorufin in Zeolite Crystals

We have used confocal laser scanning microscopy on the small, fluorescent resorufin dye molecule to visualize molecular accessibility and diffusion in the hierarchical, anisotropic pore structure of large (~10 μm-sized) zeolite-β crystals. The resorufin dye is widely used in life and materials science, but only in its deprotonated form because the protonated molecule is barely fluorescent in aqueous solution. In this work, we show that protonated resorufin is in fact strongly fluorescent when confined within zeolite micropores, thus enabling fluorescence microimaging experiments. We find that J-aggregation guest–guest interactions lead to a decrease in the measured fluorescence intensity that can be prevented by using non-fluorescent spacer molecules. We characterized the pore space by introducing resorufin from the outside solution and following its diffusion into zeolite-β crystals. The eventual homogeneous distribution of resorufin molecules throughout the zeolite indicates a fully accessible pore network. This enables the quantification of the diffusion coefficient in the straight pores of zeolite-β without the need for complex analysis, and we found a value of 3×10−15 m2 s−1. Furthermore, we saw that diffusion through the straight pores of zeolite-β is impeded when crossing the boundaries between zeolite subunits

Laboratory evolution of a glucose-phosphorylation-deficient, arabinose-fermenting S. cerevisiae strain reveals mutations in GAL2 that enable glucose-insensitive l-arabinose uptake

Cas9-assisted genome editing was used to construct an engineered glucose-phosphorylation-negative S. cerevisiae strain, expressing the Lactobacillus plantaruml-arabinose pathway and the Penicillium chrysogenum transporter PcAraT. This strain, which showed a growth rate of 0.26 h-1 on l-arabinose in aerobic batch cultures, was subsequently evolved for anaerobic growth on l-arabinose in the presence of d-glucose and d-xylose. In four strains isolated from two independent evolution experiments the galactose-transporter gene GAL2 had been duplicated, with all alleles encoding Gal2N376T or Gal2N376I substitutions. In one strain, a single GAL2 allele additionally encoded a Gal2T89I substitution, which was subsequently also detected in the independently evolved strain IMS0010. In 14C-sugar-transport assays, Gal2N376S, Gal2N376T and Gal2N376I substitutions showed a much lower glucose sensitivity of l-arabinose transport and a much higher Km for d-glucose transport than wild-type Gal2. Introduction of the Gal2N376I substitution in a non-evolved strain enabled growth on l-arabinose in the presence of d-glucose. Gal2N376T, T89I and Gal2T89I variants showed a lower Km for l-arabinose and a higher Km for d-glucose than wild-type Gal2, while reverting Gal2N376T, T89I to Gal2N376 in an evolved strain negatively affected anaerobic growth on arabinose. This study indicates that optimal conversion of mixed-sugar feedstocks may require complex 'transporter landscapes', consisting of sugar transporters with complementary kinetic and regulatory properties