Scientific publications

2014
The whole is more than the sum of all its parts: collective effect of spider attachment organs

Wohlfart, Ellen | Wolff, Jonas O. | Arzt, Eduard | Gorb, Stanislav N.

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Dynamic attachment is the key to moving safely and fast in a three-dimensional environment. Among lizards, hexapods and arachnids, several lineages have evolved hairy foot pads that can generate strong friction and adhesion on both smooth and rough surfaces. A strongly expressed directionality of attachment structures results in an anisotropy of frictional properties, which might be crucial for attachment control. In a natural situation, more than one leg is usually in contact with the substrate. In order to understand the collective effect of hairy foot pads in the hunting spider Cupiennius salei (Arachnida, Ctenidae), we performed vertical pulling experiments combined with stepwise disabling of the pads. We found the attachment force of the spider to be not simply the sum of single leg forces because with leg pair deactivation a much greater decrease in attachment forces was found than was predicted by just the loss of available adhesive pad area. This indicates that overall adhesion ability of the spider is strongly dependent on the antagonistic work of opposing legs, and the apparent contact area plays only a minor role. It is concluded that the coordinated action of the legs is crucial for adhesion control and for fast and easy detachment. The cumulative effect of anisotropic fibrillar adhesive structures could be potentially interesting for biomimetic applications, such as novel gripping devices.

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Journal of Experimental Biology,
2014, 217 (2), 222-224.

In situ experiments to reveal the role of surface feature sidewalls in the Cassie-Wenzel transition

Hensel, René | Finn, Andreas | Helbig, Ralf | Killge, Sebastian | Braun, Hans-Georg | Werner, Carsten

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Waterproof and self-cleaning surfaces continue to attract much attention as they can be instrumental in various different technologies. Such surfaces are typically rough, allowing liquids to contact only the outermost tops of their asperities, with air being entrapped underneath. The formed solid-liquid-air interface is metastable and, hence, can be forced into a completely wetted solid surface. A detailed understanding of the wetting barrier and the dynamics of this transition is critically important for the practical use of the related surfaces. Toward this aim, wetting transitions were studied in situ at a set of patterned perfluoropolyether dimethacrylate (PFPEdma) polymer surfaces exhibiting surface features with different types of sidewall profiles. PFPEdma is intrinsically hydrophobic and exhibits a refractive index very similar to water. Upon immersion of the patterned surfaces into water, incident light was differently scattered at the solid-liquid-air and solid-liquid interface, which allows for distinguishing between both wetting states by dark-field microscopy. The wetting transition observed with this methodology was found to be determined by the sidewall profiles of the patterned structures. Partial recovery of the wetting was demonstrated to be induced by abrupt and continuous pressure reductions. A theoretical model based on Laplace's law was developed and applied, allowing for the analytical calculation of the transition barrier and the potential to revert the wetting upon pressure reduction.

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Langmuir,
2014, 30 (50), 15162-15170.

OPEN ACCESS
Comparison of segregations formed in unmodified and Sr-modified Al-Si alloys studied by atom probe tomography and transmission electron microscopy

Barrirero, Jenifer | Engstler, Michael | Ghafoor, Naureen | de Jonge, Niels | Odén, Magnus | Mücklich, Frank

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The mechanical properties of Al-7 wt.% Si can be enhanced by structural modifications of its eutectic phase. Addition of low concentrations of certain elements, in this case 150 wt-ppm Sr, is enough to cause a transition from a coarse plate-like Si structure to a finer coralline one. To fully understand the operating mechanism of this modification, the composition of the eutectic Si phase in unmodified and Sr-modified alloys was analysed and compared by atom probe tomography and (scanning) transmission electron microscopy. The unmodified alloy showed nanometre sized Al-segregations decorating defects, while the Sr-modified sample presented three types of Al–Sr segregations: (1) rod-like segregations that promote smoothening of the Al–Si boundaries in the eutectic phase, (2) particle-like segregations comparable to the ones seen in the unmodified alloy, and (3) planar segregations favouring the formation of twin boundaries. Al and Sr solubilities in Si after solidification were determined to be 430 ± 160 at-ppm and 40 ± 10 at-ppm, respectively. Sr predominantly segregates to the Si phase confirming its importance in the modification of the eutectic growth.

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Journal of Alloys and Compounds,
2014, 611, 410-421.

Combined Scanning Transmission Electron Microscopy tilt- and focal series

Dahmen, Tim | Baudoin, Jean-Pierre | Lupini, Andrew R. | Kübel,Christian | Slusallek, Philipp | de Jonge, Niels

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In this study, a combined tilt- and focal series is proposed as a new recording scheme for high-angle annular dark-field scanning transmission electron microscopy (STEM) tomography. Three-dimensional (3D) data were acquired by mechanically tilting the specimen, and recording a through-focal series at each tilt direction. The sample was a whole-mount macrophage cell with embedded gold nanoparticles. The tilt-focal algebraic reconstruction technique (TF-ART) is introduced as a new algorithm to reconstruct tomograms from such combined tilt- and focal series. The feasibility of TF-ART was demonstrated by 3D reconstruction of the experimental 3D data. The results were compared with a conventional STEM tilt series of a similar sample. The combined tilt- and focal series led to smaller "missing wedge" artifacts, and a higher axial resolution than obtained for the STEM tilt series, thus improving on one of the main issues of tilt series-based electron tomography.

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Microscopy and Microanalysis,
2014, 20 (2), 548-560.

TFS: Combined tilt- and focal series scanning transmission electron microscopy

Dahmen, Tim | Baudoin, Jean-Pierre | Lupini, Andrew R. | Kübel, Christian | Slusallek, Philipp | de Jonge, Niels

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Microscopy and Microanalysis,
2014, 20 (Supplement S3), 786-787.

Introduction to special issue on electron microscopy of specimens in liquid

Microscopy and Microanalysis,
2014, 20 (2), 315-316.

Liquid scanning transmission electron microscopy: Imaging protein complexes in their native environment in whole Eukaryotic cells

Peckys, Diana B. | de Jonge, Niels

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Scanning transmission electron microscopy (STEM) of specimens in liquid, so-called Liquid STEM, is capable of imaging the individual subunits of macromolecular complexes in whole eukaryotic cells in liquid. This paper discusses this new microscopy modality within the context of state-of-the-art microscopy of cells. The principle of operation and equations for the resolution are described. The obtained images are different from those acquired with standard transmission electron microscopy showing the cellular ultrastructure. Instead, contrast is obtained on specific labels. Images can be recorded in two ways, either via STEM at 200 keV electron beam energy using a microfluidic chamber enclosing the cells, or via environmental scanning electron microscopy at 30 keV of cells in a wet environment. The first series of experiments involved the epidermal growth factor receptor labeled with gold nanoparticles. The labels were imaged in whole fixed cells with nanometer resolution. Since the cells can be kept alive in the microfluidic chamber, it is also feasible to detect the labels in unfixed, live cells. The rapid sample preparation and imaging allows studies of multiple whole cells.

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Microscopy and Microanalysis,
2014, 20 (2), 346-365.

Gold nanoparticle uptake in whole cells in liquid examined by environmental Scanning Electron Microscopy

Peckys, Diana B. | de Jonge, Niels

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The size of gold nanoparticles (AuNPs) can influence various aspects of their cellular uptake. Light microscopy is not capable of resolving most AuNPs, while electron microscopy (EM) is not practically capable of acquiring the necessary statistical data from many cells and the results may suffer from various artifacts. Here, we demonstrate the use of a fast EM method for obtaining high-resolution data from a much larger population of cells than is usually feasible with conventional EM. A549 (human lung carcinoma) cells were subjected to uptake protocols with 10, 15, or 30 nm diameter AuNPs with adsorbed serum proteins. After 20 min, 24 h, or 45 h, the cells were fixed and imaged in whole in a thin layer of liquid water with environmental scanning electron microscopy equipped with a scanning transmission electron microscopy detector. The fast preparation and imaging of 145 whole cells in liquid allowed collection of nanoscale data within an exceptionally small amount of time of ~80 h. Analysis of 1,041 AuNP-filled vesicles showed that the long-term AuNP storing lysosomes increased their average size by 80 nm when AuNPs with 30 nm diameter were uptaken, compared to lysosomes of cells incubated with AuNPs of 10 and 15 nm diameter.

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Microscopy and Microanalysis,
2014, 20 (01), 189-197.

Liquid scanning transmission electron microscopy: Nanoscale imaging in micrometers-thick liquids

Schuh, Tobias | de Jonge, Niels

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Scanning transmission electron microscopy (STEM) of specimens in liquid is possible using a microfluidic chamber with thin silicon nitride windows. This paper includes an analytic equation of the resolution as a function of the sample thickness and the vertical position of an object in the liquid. The equipment for STEM of liquid specimen is briefly described. STEM provides nanometer resolution in micrometer-thick liquid layers with relevance for both biological research and materials science. Using this technique, we investigated tagged proteins in whole eukaryotic cells, and gold nanoparticles in liquid with time-lapse image series. Possibly future applications are discussed. / La microscopie électronique à balayage en transmission (STEM) d'échantillons immergés dans un liquide est possible en utilisant une chambre microfluidique réalisée avec de fines fenêtres en nitrure de silicium. Cet article introduit d'abord une équation analytique permettant d'estimer la résolution spatiale accessible en fonction de l'épaisseur totale de l'échantillon et de la position de l'objet d'intérêt en son sein. Après une description brève de l'équipement utilisable, nous montrons comment cette approche STEM permet d'observer avec une résolution nanométrique des objets d'intérêt en biologie ou en science des matériaux, plongés dans une couche liquide de plusieurs micromètres d'épaisseur. Avec cette technique, nous avons étudié la distribution de protéines marquées dans des cellules eucaryotes complètes et celle dynamique de nanoparticules d'or dans un liquide au moyen de séries d'images résolues en temps. Enfin, nous proposons quelques grands axes pour de futures applications.

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Comptes Rendus Physique,
2014, 15 (2-3), 214-223.

The role of physical and chemical properties of Pd nanostructured materials immobilized on inorganic carriers on ion formation in atmospheric pressure laser desorption/ionization mass spectrometry

Silina, Yuliya E. | Koch, Marcus | Volmer, Dietrich A.

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Fundamental parameters influencing the ion-producing efficiency of palladium nanostructures (nanoparticles [Pd-NP], nanoflowers, nanofilms) during laser irradiation were studied in this paper. The nanostructures were immobilized on the surface of different solid inorganic carrier materials (porous and mono-crystalline silicon, anodic porous aluminum oxide, glass and polished steel) by using classical galvanic deposition, electroless local deposition and sputtering. It was the goal of this study to investigate the influence of both the nanoparticular layer as well as the carrier material on ion production for selected analyte molecules. Our experiments demonstrated that the dimensions of the synthesized nanostructures, the thickness of the active layers, surface disorders, thermal conductivity and physically or chemically adsorbed water influenced signal intensities of analyte ions during surface-assisted laser desorption/ionization (SALDI) while no effects such as plasmon resonance, photoelectric effect or catalytic activity were expected to occur. Excellent LDI abilities were seen for Pd-NPs immobilized on steel, while Pd nanoflowers on porous silicon exhibited several disadvantages; viz, strong memory effects, dependency of the analytical signal on amount of physically and chemically adsorbed water inside porous carrier, reduced SALDI activity from unstable connections between Pd and semiconductor material, decrease of the melting point of pure silicon after Pd immobilization and resulting strong laser ablation of metal/semiconductor complex, as well as significantly changed surface morphology after laser irradiation. The analytical performance of Pd-NP/steel was further improved by applying a hydrophobic coating to the steel surface before galvanic deposition. This procedure increased the distance between Pd-NPs, thus reducing thermal stress upon LDI; it simultaneously decreased spot sizes of deposited sample solutions.

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Journal of Mass Spectrometry,
2014, 49 (6), 468-480.