Browsing by Author "Bennewitz, Roland"
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- ItemBending as Key Mechanism in the Tactile Perception of Fibrillar Surfaces(Weinheim : Wiley-VCH, 2021) Gedsun, Angelika; Sahli, Riad; Meng, Xing; Hensel, René; Bennewitz, RolandThe touching of fibrillar surfaces elicits a broad range of affective reactions, which range from the adverse stinginess of a stiff bristle brush to the pleasant feel of velvet. To study the tactile perception of model fibrillar surfaces, a unique set of samples carrying dense, regular arrays of cylindrical microfibrils with high aspect ratio made from different elastomer materials have been created. Fibril length and material compliance are varied independently such that their respective influence on tactile perception can be elucidated. This work finds that the tactile perception of similarity between samples is dominated by bending of the fibrils under sliding touch. The results demonstrate that variations of material stiffness and of surface structure are not necessarily perceived independently by touch. In the case of fibrillar elastomer surfaces, it is rather the ratio of fibril length and storage modulus which determines fibril bending and becomes the dominant tactile dimension. Visual access to the sample during tactile exploration improves the tactile perception of fibril bendability. Experiments with colored samples show a distraction by color in participants’ decisions regarding tactile similarity only for yellow samples of outstanding brightness.
- ItemDischarge during detachment of micro-structured PDMS sheds light on the role of electrostatics in adhesion(Milton Park : Taylor & Francis, 2012) Brörmann, Katrin; Burger, Karin; Jagota, Anand; Bennewitz, RolandLight emission due to discharge in air is detected during and after the detachment of microstructured PDMS samples from glass surfaces, showing contact charging of the surfaces. The light emission provides information about the detachment process, like the velocity of the peeling front, which is difficult to obtain otherwise. While the work of separation exhibits the dependence on pulling velocity typically found for viscoelastic materials, the emission intensity exhibits almost no velocity dependence. We present a model for the rate-dependent contribution of a mosaic of contact charges to the work of separation. Also, the work of separation increases as expected with increasing aspect ratio of the microstructure, while the emission intensity shows a maximum for intermediate structures. Based on their different dependencies and on an upper-bound estimate of the energy emitted as light, we conclude that for the given system the contribution of electrostatic attraction to the work of separation is minor.
- ItemDynamic effects in friction and adhesion through cooperative rupture and formation of supramolecular bonds(Cambridge : Royal Society of Chemistry, 2015) Blass, Johanna; Albrecht, Marcel; Bozna, Bianca L.; Wenz, Gerhard; Bennewitz, RolandWe introduce a molecular toolkit for studying the dynamics in friction and adhesion from the single molecule level to effects of multivalency. As experimental model system we use supramolecular bonds established by the inclusion of ditopic adamantane connector molecules into two surface-bound cyclodextrin molecules, attached to a tip of an atomic force microscope (AFM) and to a flat silicon surface. The rupture force of a single bond does not depend on the pulling rate, indicating that the fast complexation kinetics of adamantane and cyclodextrin are probed in thermal equilibrium. In contrast, the pull-off force for a group of supramolecular bonds depends on the unloading rate revealing a non-equilibrium situation, an effect discussed as the combined action of multivalency and cantilever inertia effects. Friction forces exhibit a stick-slip characteristic which is explained by the cooperative rupture of groups of host-guest bonds and their rebinding. No dependence of friction on the sliding velocity has been observed in the accessible range of velocities due to fast rebinding and the negligible delay of cantilever response in AFM lateral force measurements.
- ItemFingertip friction and tactile rating of wrapping papers(Berlin ; Heidelberg : Springer, 2022) Jost, Kim Michèle; Drewing, Knut; Bennewitz, Roland; Seifi, Hasti; Kappers, Astrid M. L.; Schneider, Oliver; Drewing, Knut; Pacchierotti, Claudio; Abbasimoshaei, Alireza; Huisman, Gijs; Kern, Thorsten A.The tactile exploration and perception of wrapping papers is investigated in terms of fingertip friction and rating of sensory, affective, and evaluative adjectives. Friction coefficients, which vary significantly between samples, are correlated with factors such as valence which are identified in a principal component analysis of subjective ratings. We found that affective appraisals of valence and arousal as well as evaluations of novelty, but not of value, decreased with increasing friction.
- ItemForce microscopy of layering and friction in an ionic liquid(Bristol : IOP Publishing, 2014) Hoth, Judith; Hausen, Florian; Müser, Martin H.; Bennewitz, RolandThe mechanical properties of the ionic liquid 1-butyl-1-methylpyrrolidinium tris(pentafluoroethyl) trifluorophosphate ([Py1,4][FAP]) in confinement between a SiOx and a Au(1 1 1) surface are investigated by means of atomic force microscopy (AFM) under electrochemical control. Up to 12 layers of ion pairs can be detected through force measurements while approaching the tip of the AFM to the surface. The particular shape of the force versus distance curve is explained by a model for the interaction between tip, gold surface and ionic liquid, which assumes an exponentially decaying oscillatory force originating from bulk liquid density correlations. Jumps in the tip–sample distance upon approach correspond to jumps of the compliant force sensor between branches of the oscillatory force curve. Frictional force between the laterally moving tip and the surface is detected only after partial penetration of the last double layer between tip and surface.
- ItemFormation of intermittent covalent bonds at high contact pressure limits superlow friction on epitaxial graphene(College Park, MD : APS, 2023) Szczefanowicz, Bartosz; Kuwahara, Takuya; Filleter, Tobin; Klemenz, Andreas; Mayrhofer, Leonhard; Bennewitz, Roland; Moseler, MichaelEpitaxial graphene on SiC(0001) exhibits superlow friction due to its weak out-of-plane interactions. Friction-force microscopy with silicon tips shows an abrupt increase of friction by one order of magnitude above a threshold normal force. Density-functional tight-binding simulations suggest that this wearless high-friction regime involves an intermittent sp3 rehybridization of graphene at contact pressure exceeding 10 GPa. The simultaneous formation of covalent bonds with the tip's silica surface and the underlying SiC interface layer establishes a third mechanism limiting the superlow friction on epitaxial graphene, in addition to dissipation in elastic instabilities and in wear processes.
- ItemFriction force microscopy of tribochemistry and interfacial ageing for the SiOx/Si/Au system(Frankfurt am Main : Beilstein-Institut, 2018) Petzhold, Chritinane; Koch, Marcus; Bennewitz, RolandFriction force microscopy was performed with oxidized or gold-coated silicon tips sliding on Au(111) or oxidized Si(100) surfaces in ultrahigh vacuum. We measured very low friction forces compared to adhesion forces and found a modulation of lateral forces reflecting the atomic structure of the surfaces. Holding the force-microscopy tip stationary for some time did not lead to an increase in static friction, i.e., no contact ageing was observed for these pairs of tip and surface. Passivating layers from tip or surface were removed in order to allow for contact ageing through the development of chemical bonds in the static contact. After removal of the passivating layers, tribochemical reactions resulted in strong friction forces and tip wear. Friction, wear, and the re-passivation by oxides are discussed based on results for the temporal development of friction forces, on images of the scanned area after friction force microscopy experiments, and on electron microscopy of the tips.
- ItemFriction mediated by redox-active supramolecular connector molecules(Washington D.C. : American Chemical Society, 2015) Bozna, Bianca L.; Blass, Johanna; Albrecht, Marcel; Hausen, Florian; Wenz, Gerhard; Bennewitz, RolandWe report on a friction study at the nanometer scale using atomic force microscopy under electrochemical control. Friction arises from the interaction between two surfaces functionalized with cyclodextrin molecules. The interaction is mediated by connector molecules with (ferrocenylmethyl)ammonium end groups forming supramolecular complexes with the cyclodextrin molecules. With ferrocene connector molecules in solution, the friction increases by a factor of up to 12 compared to control experiments without connector molecules. The electrochemical oxidation of ferrocene to ferrocenium causes a decrease in friction owing to the lower stability of ferrocenium−cyclodextrin complex. Upon switching between oxidative and reduction potentials, a change in friction by a factor of 1.2−1.8 is observed. Isothermal titration calorimetry reveals fast dissociation and rebinding kinetics and thus an equilibrium regime for the friction experiments.
- ItemHuman glabrous skin contains crystallized urea dendriform structures in the stratum corneum which affect the hydration levels(Oxford : Wiley-Blackwell, 2023) Infante, Victor Hugo Pacagnelli; Bennewitz, Roland; Kröger, Marius; Meinke, Martina C.; Darvin, Maxim E.Glabrous skin is hair-free skin with a high density of sweat glands, which is found on the palms, and soles of mammalians, covered with a thick stratum corneum. Dry hands are often an occupational problem which deserves attention from dermatologists. Urea is found in the skin as a component of the natural moisturizing factor and of sweat. We report the discovery of dendrimer structures of crystalized urea in the stratum corneum of palmar glabrous skin using laser scanning microscopy. The chemical and structural nature of the urea crystallites was investigated in vivo by non-invasive techniques. The relation of crystallization to skin hydration was explored. We analysed the index finger, small finger and tenar palmar area of 18 study participants using non-invasive optical methods, such as laser scanning microscopy, Raman microspectroscopy and two-photon tomography. Skin hydration was measured using corneometry. Crystalline urea structures were found in the stratum corneum of about two-thirds of the participants. Participants with a higher density of crystallized urea structures exhibited a lower skin hydration. The chemical nature and the crystalline structure of the urea were confirmed by Raman microspectroscopy and by second harmonic generated signals in two-photon tomography. The presence of urea dendrimer crystals in the glabrous skin seems to reduce the water binding capacity leading to dry hands. These findings highlight a new direction in understanding the mechanisms leading to dry hands and open opportunities for the development of better moisturizers and hand disinfection products and for diagnostic of dry skin.
- ItemImportance of surface oxide for the tribology of a Zr-based metallic glass(Heidelberg : Springer, 2017) Kang, S.J.; Rittig, Kai Thomas; Kwan, S.G.; Park, H.W.; Bennewitz, Roland; Caron, ArnaudThermally grown surface oxide layers dominate the single-asperity tribological behavior of a Zr60Cu30Al10 glass. Increase in oxidation time leads to an increased contribution of shearing and a corresponding decreased contribution of ploughing to friction. This change in the dominating friction and wear mechanism results in an overall minor decrease of the friction coefficient of oxidized surfaces compared to the metallic glass sample with native surface oxide. Our results demonstrate the importance of creating a stable oxide layer for practical applications of metallic glasses in micro-devices involving sliding contact.
- ItemIn Situ Observation Reveals Local Detachment Mechanisms and Suction Effects in Micropatterned Adhesives(Weinheim : Wiley-VCH, 2019) Tinnemann, Verena; Hernández, Luissé; Fischer, Sarah C.L.; Arzt, Eduard; Bennewitz, Roland; Hensel, RenéFibrillar adhesion pads of insects and geckoes have inspired the design of high-performance adhesives enabling a new generation of handling devices. Despite much progress over the last decade, the current understanding of these adhesives is limited to single contact pillars and the behavior of whole arrays is largely unexplored. In the study reported here, a novel approach is taken to gain insight into the detachment mechanisms of whole micropatterned arrays. Individual contacts are imaged by frustrated total internal reflection, allowing in situ observation of contact formation and separation during adhesion tests. The detachment of arrays is found to be governed by the distributed adhesion strength of individual pillars, but no collaborative effect mediated by elastic interactions can be detected. At the maximal force, about 30% of the mushroom structures are already detached. The adhesive forces decrease with reduced air pressure by 20% for the smooth and by 6% for the rough specimen. These contributions are attributed to a suction effect, whose strength depends critically on interfacial defects controlling the sealing quality of the contact. This dominates the detachment process and the resulting adhesion strength. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemInteractions between shape-persistent macromolecules as probed by AFM(Frankfurt am Main : Beilstein-Institut, 2017) Blas, Johannes; Brunke, Jessica; Emmerich, Franziska; Cédric, Przybylski; Garamus, Vasil M.; Feoktystov, Artem; Bennewitz, Roland; Wenz, Gerhard; Albrecht, MarcelWater-soluble shape-persistent cyclodextrin (CD) polymers with amino-functionalized end groups were prepared starting from diacetylene-modified cyclodextrin monomers by a combined Glaser coupling/click chemistry approach. Structural perfection of the neutral CD polymers and inclusion complex formation with ditopic and monotopic guest molecules were proven by MALDI–TOF and UV–vis measurements. Small-angle neutron and X-ray (SANS/SAXS) scattering experiments confirm the stiffness of the polymer chains with an apparent contour length of about 130 Å. Surface modification of planar silicon wafers as well as AFM tips was realized by covalent bound formation between the terminal amino groups of the CD polymer and a reactive isothiocyanate–silane monolayer. Atomic force measurements of CD polymer decorated surfaces show enhanced supramolecular interaction energies which can be attributed to multiple inclusion complexes based on the rigidity of the polymer backbone and the regular configuration of the CD moieties. Depending on the geometrical configuration of attachment anisotropic adhesion characteristics of the polymer system can be distinguished between a peeling and a shearing mechanism.
- ItemKelvin probe force microscopy of charged indentation-induced dislocation structures in KBr(Saarbrücken : Leibniz-Institut für neue Materialien, 2009) Egberts, Philip; Bennewitz, RolandThe incipient stages of plasticity in KBr single crystals have been examined in ultrahigh vacuum by means of Atomic Force Microscopy and Kelvin Probe Force Microscopy (KPFM). Conducting diamond-coated tips have been used to both indent the crystals and image the resulting plastic deformation. KPFM reveals that edge dislocations intersecting the surface carry a negative charge similar to kinks in surface steps, while screw dislocations show no contrast. Weak topographic features extending in <110> direction from the indentation are identified by atomic-resolution imaging to be pairs of edge dislocations of opposite sign, separated by a distance similar to the indenter radius. They indicate the glide of two parallel {110} planes perpendicular to the surface, a process that allows for a slice of KBr to be pushed away from the indentation site.
- ItemLike a Second Skin: Understanding How Epidermal Devices Affect Human Tactile Perception(New York,NY,United States : Association for Computing Machinery, 2019) Nittala, Aditya Shekhar; Kruttwig, Klaus; Lee, Jaeyeon; Bennewitz, Roland; Arzt, Eduard; Steimle, Jürgen; Brewster, StephenThe emerging class of epidermal devices opens up new opportunities for skin-based sensing, computing, and interaction. Future design of these devices requires an understanding of how skin-worn devices affect the natural tactile perception. In this study, we approach this research challenge by proposing a novel classification system for epidermal devices based on flexural rigidity and by testing advanced adhesive materials, including tattoo paper and thin films of poly (dimethylsiloxane) (PDMS). We report on the results of three psychophysical experiments that investigated the effect of epidermal devices of different rigidity on passive and active tactile perception. We analyzed human tactile sensitivity thresholds, two-point discrimination thresholds, and roughness discrimination abilities on three different body locations (fingertip, hand, forearm). Generally, a correlation was found between device rigidity and tactile sensitivity thresholds as well as roughness discrimination ability. Surprisingly, thin epidermal devices based on PDMS with a hundred times the rigidity of commonly used tattoo paper resulted in comparable levels of tactile acuity. The material offers the benefit of increased robustness against wear and the option to re-use the device. Based on our findings, we derive design recommendations for epidermal devices that combine tactile perception with device robustness.
- ItemLower nanometer-scale size limit for the deformation of a metallic glass by shear transformations revealed by quantitative AFM indentation(Frankfurt am Main : Beilstein-Institut, 2015) Caron, Arnaud; Bennewitz, RolandWe combine non-contact atomic force microscopy (AFM) imaging and AFM indentation in ultra-high vacuum to quantitatively and reproducibly determine the hardness and deformation mechanisms of Pt(111) and a Pt57.5Cu14.7Ni5.3P22.5 metallic glass with unprecedented spatial resolution. Our results on plastic deformation mechanisms of crystalline Pt(111) are consistent with the discrete mechanisms established for larger scales: Plasticity is mediated by dislocation gliding and no rate dependence is observed. For the metallic glass we have discovered that plastic deformation at the nanometer scale is not discrete but continuous and localized around the indenter, and does not exhibit rate dependence. This contrasts with the observation of serrated, rate-dependent flow of metallic glasses at larger scales. Our results reveal a lower size limit for metallic glasses below which shear transformation mechanisms are not activated by indentation. In the case of metallic glass, we conclude that the energy stored in the stressed volume during nanometer-scale indentation is insufficient to account for the interfacial energy of a shear band in the glassy matrix.
- ItemMolecular stiffness cues of an interpenetrating network hydrogel for cell adhesion(Amsterdam : Elsevier, 2022) Li, Bin; Çolak, Arzu; Blass, Johanna; Han, Mitchell; Zhang, Jingnan; Zheng, Yijun; Jiang, Qiyang; Bennewitz, Roland; del Campo, AránzazuUnderstanding cells' response to the macroscopic and nanoscale properties of biomaterials requires studies in model systems with the possibility to tailor their mechanical properties and different length scales. Here, we describe an interpenetrating network (IPN) design based on a stiff PEGDA host network interlaced within a soft 4-arm PEG-Maleimide/thiol (guest) network. We quantify the nano- and bulk mechanical behavior of the IPN and the single network hydrogels by single-molecule force spectroscopy and rheological measurements. The IPN presents different mechanical cues at the molecular scale, depending on which network is linked to the probe, but the same mechanical properties at the macroscopic length scale as the individual host network. Cells attached to the interpenetrating (guest) network of the IPN or to the single network (SN) PEGDA hydrogel modified with RGD adhesive ligands showed comparable attachment and spreading areas, but cells attached to the guest network of the IPN, with lower molecular stiffness, showed a larger number and size of focal adhesion complexes and a higher concentration of the Hippo pathway effector Yes-associated protein (YAP) than cells linked to the PEGDA single network. The observations indicate that cell adhesion to the IPN hydrogel through the network with lower molecular stiffness proceeds effectively as if a higher ligand density is offered. We claim that IPNs can be used to decipher how changes in ECM design and connectivity at the local scale affect the fate of cells cultured on biomaterials.
- ItemNanomechanics of self-assembled DNA building blocks(Cambridge : RSC Publ., 2021) Penth, Michael; Schellnhuber, Kordula; Bennewitz, Roland; Blass, JohannaDNA has become a powerful platform to design functional nanodevices. DNA nanodevices are often composed of self-assembled DNA building blocks that differ significantly from the structure of native DNA. In this study, we present Flow Force Microscopy as a massively parallel approach to study the nanomechanics of DNA self-assemblies on the single-molecular level. The high-throughput experiments performed in a simple microfluidic channel enable statistically meaningful studies with nanometer scale precision in a time frame of several minutes. A surprisingly high flexibility was observed for a typical construct used in DNA origami, reflected in a persistence length of 10.2 nm, a factor of five smaller than for native DNA. The enhanced flexibility is attributed to the discontinuous backbone of DNA self-assemblies that facilitate base pair opening by thermal fluctuations at the end of hybridized oligomers. We believe that the results will contribute to the fundamental understanding of DNA nanomechanics and help to improve the design of DNA nanodevices with applications in biological analysis and clinical research.
- ItemNanoscale friction on MoS2/graphene heterostructures(Cambridge : RSC Publ., 2023) Liu, Zhao; Szczefanowicz, Bartosz; Lopes, J. Marcelo J.; Gan, Ziyang; George, Antony; Turchanin, Andrey; Bennewitz, RolandStacked hetero-structures of two-dimensional materials allow for a design of interactions with corresponding electronic and mechanical properties. We report structure, work function, and frictional properties of 1 to 4 layers of MoS2 grown by chemical vapor deposition on epitaxial graphene on SiC(0001). Experiments were performed by atomic force microscopy in ultra-high vacuum. Friction is dominated by adhesion which is mediated by a deformation of the layers to adapt the shape of the tip apex. Friction decreases with increasing number of MoS2 layers as the bending rigidity leads to less deformation. The dependence of friction on applied load and bias voltage can be attributed to variations in the atomic potential corrugation of the interface, which is enhanced by both load and applied bias. Minimal friction is obtained when work function differences are compensated.
- ItemOptoregulated force application to cellular receptors using molecular motors(London : Nature Publishing Group, 2021) Zheng, Yijun; Han, Mitchell K.L.; Zhao, Renping; Blass, Johanna; Zhang, Jingnan; Zhou, Dennis W.; Colard-Itté, Jean-Rémy; Dattler, Damien; Çolak, Arzu; Hoth, Markus; García, Andrés J.; Qu, Bin; Bennewitz, Roland; Giuseppone, Nicolas; del Campo, AránzazuProgress in our understanding of mechanotransduction events requires noninvasive methods for the manipulation of forces at molecular scale in physiological environments. Inspired by cellular mechanisms for force application (i.e. motor proteins pulling on cytoskeletal fibers), we present a unique molecular machine that can apply forces at cell-matrix and cell-cell junctions using light as an energy source. The key actuator is a light-driven rotatory molecular motor linked to polymer chains, which is intercalated between a membrane receptor and an engineered biointerface. The light-driven actuation of the molecular motor is converted in mechanical twisting of the entangled polymer chains, which will in turn effectively “pull” on engaged cell membrane receptors (e.g., integrins, T cell receptors) within the illuminated area. Applied forces have physiologically-relevant magnitude and occur at time scales within the relevant ranges for mechanotransduction at cell-friendly exposure conditions, as demonstrated in force-dependent focal adhesion maturation and T cell activation experiments. Our results reveal the potential of nanomotors for the manipulation of living cells at the molecular scale and demonstrate a functionality which at the moment cannot be achieved by other technologies for force application.
- ItemPerception of Friction in Tactile Exploration of Micro-structured Rubber Samples(Berlin ; Heidelberg : Springer, 2022) Fehlberg, Maja; Kim, Kwang-Seop; Drewing, Knut; Hensel, René; Bennewitz, Roland; Seifi, Hasti; Kappers, Astrid M. L.; Schneider, Oliver; Drewing, Knut; Pacchierotti, Claudio; Abbasimoshaei, Alireza; Huisman, Gijs; Kern, Thorsten A.Fingertip friction and the related shear of skin are key mechanical mechanisms in tactile perception, but the perception of friction itself is rarely explored except for the flat surfaces of tactile displays. We investigated the perception of friction for tactile exploration of a unique set of samples whose fabric-like surfaces are equipped with regular arrays of flexible micropillars. The measured fingertip friction increases with decreasing bending stiffness, where the latter is controlled by radius (20–75 µm) and aspect ratio of the micropillars. In forced-choice tasks, participants noticed relative differences in friction as small as 0.2, and even smaller when a sample with less than 100 µm distance between pillars is omitted from the analysis. In an affective ranking of samples upon active touch, the perception of pleasantness is anticorrelated with the measured friction. Our results offer insights towards a rational design of materials with well-controlled surface microstructure which elicit a dedicated tactile appeal.