O-glycans Expand Lubricin and Attenuate Its Viscosity and Shear Thinning.

Lubricin, an intrinsically disordered glycoprotein, plays a pivotal role in facilitating smooth movement and ensuring the enduring functionality of synovial joints. The central domain of this protein serves as a source of this excellent lubrication and is characterized by its highly glycosylated, negatively charged, and disordered structure. However, the influence of O-glycans on the viscosity of lubricin remains unclear. In this study, we employ molecular dynamics simulations in the absence and presence of shear, along with continuum simulations, to elucidate the intricate interplay between O-glycans and lubricin and the impact of O-glycans on lubricin's conformational properties and viscosity. We found the presence of O-glycans to induce a more extended conformation in fragments of the disordered region of lubricin. These O-glycans contribute to a reduction in solution viscosity but at the same time weaken shear thinning at high shear rates, compared to nonglycosylated systems with the same density. This effect is attributed to the steric and electrostatic repulsion between the fragments, which prevents their conglomeration and structuring. Our computational study yields a mechanistic mechanism underlying previous experimental observations of lubricin and paves the way to a more rational understanding of its function in the synovial fluid.

Programmable gear-based mechanical metamaterials.

Elastic properties of classical bulk materials can hardly be changed or adjusted in operando, while such tunable elasticity is highly desired for robots and smart machinery. Although possible in reconfigurable metamaterials, continuous tunability in existing designs is plagued by issues such as structural instability, weak robustness, plastic failure and slow response. Here we report a metamaterial design paradigm using gears with encoded stiffness gradients as the constituent elements and organizing gear clusters for versatile functionalities. The design enables continuously tunable elastic properties while preserving stability and robust manoeuvrability, even under a heavy load. Such gear-based metamaterials enable excellent properties such as continuous modulation of Young's modulus by two orders of magnitude, shape morphing between ultrasoft and solid states, and fast response. This allows for metamaterial customization and brings fully programmable materials and adaptive robots within reach.

Confinement-Induced Diffusive Sound Transport in Nanoscale Fluidic Channels.

Molecular dynamics (MD) simulations have been widely used to study flow at molecular scales. Most of this work is devoted to study the departure from continuum fluid mechanics as the confining dimension decreases. Here, we present MD results under conditions where hydrodynamic descriptions typically apply, but focus on the influence of in-plane wavelengths. Probing the long wavelength limit in thermodynamic equilibrium, we observed anomalous relaxation of the density and longitudinal momentum fluctuations. The limiting behavior can be described by an effective continuum theory that describes a transition to overdamped sound relaxation for compressible fluids.

Correlated Study of Material Interaction Between Capillary Printed Eutectic Gallium Alloys and Gold Electrodes.

Liquid metals (LMs) play a growing role in flexible electronics and connected applications. Here, LMs come into direct contact with metal electrodes thus allowing for corrosion and additional alloying, potentially compromising device stability. Nevertheless, comprehensive studies on the interfacial interaction of the materials are still sparse. Therefore, a correlated material interaction study of capillary-printed Galinstan (eutetic alloy of Ga/In/Sn) with gold surfaces and electrodes is conducted. Comprehensive application of optical microscopy, vertical scanning interferometry, scanning electron microscopy/spectroscopy, x-ray photon spectroscopy, and atomic force microscopy allow for an in depth characterization of the spreading process of LM lines on gold films, revealing the differential spread of the different LM components and the formation of intermetallic nanostructures on the surface of the surrounding gold film. A model for the growth process based on the penetration of LM along the gold film grain boundaries is proposed based on the obtained time-dependent characterization. The distribution of gold, Galinstan, and intermetallic phases in a gold wire dipped into LM is observed using X-ray nano tomography as a complementary view on the internal nanostructure. Finally, resistance measurements on LM lines connecting gold electrodes over time allow to estimate the influence on the material interaction on electronic applications.

The evolving quality of frictional contact with graphene.

Graphite and other lamellar materials are used as dry lubricants for macroscale metallic sliding components and high-pressure contacts. It has been shown experimentally that monolayer graphene exhibits higher friction than multilayer graphene and graphite, and that this friction increases with continued sliding, but the mechanism behind this remains subject to debate. It has long been conjectured that the true contact area between two rough bodies controls interfacial friction. The true contact area, defined for example by the number of atoms within the range of interatomic forces, is difficult to visualize directly but characterizes the quantity of contact. However, there is emerging evidence that, for a given pair of materials, the quality of the contact can change, and that this can also strongly affect interfacial friction. Recently, it has been found that the frictional behaviour of two-dimensional materials exhibits traits unlike those of conventional bulk materials. This includes the abovementioned finding that for few-layer two-dimensional materials the static friction force gradually strengthens for a few initial atomic periods before reaching a constant value. Such transient behaviour, and the associated enhancement of steady-state friction, diminishes as the number of two-dimensional layers increases, and was observed only when the two-dimensional material was loosely adhering to a substrate. This layer-dependent transient phenomenon has not been captured by any simulations. Here, using atomistic simulations, we reproduce the experimental observations of layer-dependent friction and transient frictional strengthening on graphene. Atomic force analysis reveals that the evolution of static friction is a manifestation of the natural tendency for thinner and less-constrained graphene to re-adjust its configuration as a direct consequence of its greater flexibility. That is, the tip atoms become more strongly pinned, and show greater synchrony in their stick-slip behaviour. While the quantity of atomic-scale contacts (true contact area) evolves, the quality (in this case, the local pinning state of individual atoms and the overall commensurability) also evolves in frictional sliding on graphene. Moreover, the effects can be tuned by pre-wrinkling. The evolving contact quality is critical for explaining the time-dependent friction of configurationally flexible interfaces.

Variations in strain affect friction and microstructure evolution in copper under a reciprocating tribological load.

The microstructure of the materials constituting a metallic frictional contact strongly influence tribological performance. Being able to tailor friction and wear is challenging due to the complex microstructure evolution associated with tribological loading. Here, we investigate the effect of the strain distribution on these processes. High-purity copper plates were morphologically surface textured with two parallel rectangles - referred to as membranes - over the entire sample length by micro-milling. By keeping the width of these membranes constant and only varying their height, reciprocating tribological loading against sapphire discs resulted in different elastic and plastic strains. Finite element simulations were carried out to evaluate the strain distribution in the membranes. It was found that the maximum elastic strain increases with decreasing membrane stiffness. The coefficient of friction decreases with increasing membrane aspect ratio. By analyzing the microstructure and local crystallographic orientation, we found that both show less change with decreasing membrane stiffness.

Wear-resistant CoCrNi multi-principal element alloy at cryogenic temperature.

Traditional high strength engineering alloys suffer from serious surface brittleness and inferior wear performance when servicing under sliding contact at cryogenic temperature. Here, we report that the recently emerging CoCrNi multi-principal element alloy defies this trend and presents dramatically enhanced wear resistance when temperature decreases from 273 to 153 K, surpassing those of cryogenic austenitic steels. The temperature-dependent structure characteristics and deformation mechanisms influencing the cryogenic wear resistance of CoCrNi are clarified through microscopic observation and atomistic simulation. It is found that sliding-induced subsurface structures show distinct scenarios at different deformation temperatures. At cryogenic condition, significant grain refinement and a deep plastic zone give rise to an extended microstructural gradient below the surface, which can accommodate massive sliding deformation, in direct contrast to the strain localization and delamination at 273 K. Meanwhile, the temperature-dependent cryogenic deformation mechanisms (stacking fault networks and phase transformation) also provide additional strengthening and toughening of the subsurface material. These features make the CoCrNi alloy particularly wear resistant at cryogenic conditions and an excellent candidate for safety-critical applications.

Materials fatigue prediction using graph neural networks on microstructure representations.

The local prediction of fatigue damage within polycrystals in a high-cycle fatigue setting is a long-lasting and challenging task. It requires identifying grains tending to accumulate plastic deformation under cyclic loading. We address this task by transcribing ferritic steel microtexture and damage maps from experiments into a microstructure graph. Here, grains constitute graph nodes connected by edges whenever grains share a common boundary. Fatigue loading causes some grains to develop slip markings, which can evolve into microcracks and lead to failure. This data set enables applying graph neural network variants on the task of binary grain-wise damage classification. The objective is to identify suitable data representations and models with an appropriate inductive bias to learn the underlying damage formation causes. Here, graph convolutional networks yielded the best performance with a balanced accuracy of 0.72 and a F1-score of 0.34, outperforming phenomenological crystal plasticity (+ 68%) and conventional machine learning (+ 17%) models by large margins. Further, we present an interpretability analysis that highlights the grains along with features that are considered important by the graph model for the prediction of fatigue damage initiation, thus demonstrating the potential of such techniques to reveal underlying mechanisms and microstructural driving forces in critical grain ensembles.

Anisotropic mechanical amorphization drives wear in diamond.

Diamond is the hardest material on Earth. Nevertheless, polishing diamond is possible with a process that has remained unaltered for centuries and is still used for jewellery and coatings: the diamond is pressed against a rotating disc with embedded diamond grit. When polishing polycrystalline diamond, surface topographies become non-uniform because wear rates depend on crystal orientations. This anisotropy is not fully understood and impedes diamond's widespread use in applications that require planar polycrystalline films, ranging from cutting tools to confinement fusion. Here, we use molecular dynamics to show that polished diamond undergoes an sp(3)-sp(2) order-disorder transition resulting in an amorphous adlayer with a growth rate that strongly depends on surface orientation and sliding direction, in excellent correlation with experimental wear rates. This anisotropy originates in mechanically steered dissociation of individual crystal bonds. Similarly to other planarization processes, the diamond surface is chemically activated by mechanical means. Final removal of the amorphous interlayer proceeds either mechanically or through etching by ambient oxygen.

A deep learning approach for complex microstructure inference.

Automated, reliable, and objective microstructure inference from micrographs is essential for a comprehensive understanding of process-microstructure-property relations and tailored materials development. However, such inference, with the increasing complexity of microstructures, requires advanced segmentation methodologies. While deep learning offers new opportunities, an intuition about the required data quality/quantity and a methodological guideline for microstructure quantification is still missing. This, along with deep learning's seemingly intransparent decision-making process, hampers its breakthrough in this field. We apply a multidisciplinary deep learning approach, devoting equal attention to specimen preparation and imaging, and train distinct U-Net architectures with 30-50 micrographs of different imaging modalities and electron backscatter diffraction-informed annotations. On the challenging task of lath-bainite segmentation in complex-phase steel, we achieve accuracies of 90% rivaling expert segmentations. Further, we discuss the impact of image context, pre-training with domain-extrinsic data, and data augmentation. Network visualization techniques demonstrate plausible model decisions based on grain boundary morphology.

Atomically smooth stress-corrosion cleavage of a hydrogen-implanted crystal.

We present a quantum-accurate multiscale study of how hydrogen-filled discoidal "platelet" defects grow inside a silicon crystal. Dynamical simulations of a 10-nm-diameter platelet reveal that H2 molecules form at its internal surfaces, diffuse, and dissociate at its perimeter, where they both induce and stabilize the breaking up of highly stressed silicon bonds. A buildup of H2 internal pressure is neither needed for nor allowed by this stress-corrosion growth mechanism, at odds with previous models. Slow platelet growth up to micrometric sizes is predicted as a consequence, making atomically smooth crystal cleavage possible in implantation experiments.

Towards programmable friction: control of lubrication with ionic liquid mixtures by automated electrical regulation.

For mechanical systems in relative motion it would be fascinating if a non-mechanical stimulus could be used to directly control friction conditions. Therefore, different combinations of lubricants and external triggers for tribological influence have already been investigated. We show that when two metallic friction partners are lubricated with ionic liquid mixtures (ILM), consisting of long-chain cation and two different high charge/mass ratio anion containing ILs, the application of an electric impulse induces a permanent change of the frictional response. Such mixtures are able to alter the coefficient of friction (COF) to a greater extent, more accurately and faster than the respective single-component ILs. This change in the frictional properties is presumably due to changes in the externally induced electrical polarization at the surface, which influences the molecular adsorption, the exchange of adsorbed ions and their molecular orientation. The correlation between surface charges and friction can be used to control friction. This is achieved by implementing an electric tribo-controller which can adjust preset friction values over time. Programming friction in this way is a first step towards tribosystems that automatically adapt to changing conditions.

Solids Under Extreme Shear: Friction-Mediated Subsurface Structural Transformations.

Tribological contacts consume a significant amount of the world's primary energy due to friction and wear in different products from nanoelectromechanical systems to bearings, gears, and engines. The energy is largely dissipated in the material underneath the two surfaces sliding against each other. This subsurface material is thereby exposed to extreme amounts of shear deformation and often forms layered subsurface microstructures with reduced grain size. Herein, the elementary mechanisms for the formation of subsurface microstructures are elucidated by systematic model experiments and discrete dislocation dynamics simulations in dry frictional contacts. The simulations show how pre-existing dislocations transform into prismatic dislocation structures under tribological loading. The stress field under a moving spherical contact and the crystallographic orientation are crucial for the formation of these prismatic structures. Experimentally, a localized dislocation structure at a depth of ≈100-150 nm is found already after the first loading pass. This dislocation structure is shown to be connected to the inhomogeneous stress field under the moving contact. The subsequent microstructural transformations and the mechanical properties of the surface layer are determined by this structure. These results hold promise at guiding material selection and alloy development for tribological loading, yielding materials tailored for specific tribological scenarios.

Boundary lubrication of heterogeneous surfaces and the onset of cavitation in frictional contacts.

Surfaces can be slippery or sticky depending on surface chemistry and roughness. We demonstrate in atomistic simulations that regular and random slip patterns on a surface lead to pressure excursions within a lubricated contact that increase quadratically with decreasing contact separation. This is captured well by a simple hydrodynamic model including wall slip. We predict with this model that pressure changes for larger length scales and realistic frictional conditions can easily reach cavitation thresholds and significantly change the load-bearing capacity of a contact. Cavitation may therefore be the norm, not the exception, under boundary lubrication conditions.

Molecular Dynamic Simulation of Collision-Induced Third-Body Formation in Hydrogen-Free Diamond-Like Carbon Asperities.

The collision of two cylindrical hydrogen-free diamond-like carbon (DLC) asperities with approximately 60 % sp3 hybridization has been studied using classical molecular dynamics. The severity of the collision can be controlled by the impact parameter b that measures the width of the projected overlap of the two cylinders. For a cylinder radius of R = 23 nm, three collisions with b = 0.5 nm, b = 1 nm and b = 2.0 nm are compared. While for the two small b a single shear band between the collision partners and a strongly localized sp2/sp1 hybridised third-body zone between the asperities is observed, the b = 2 nm collision is accompanied by pronounced plastic deformation in both asperities that destabilize the metastable sp3-rich phase leading to a drastic increase in the amount of rehybridized tribomaterial. In addition, pronounced roughening of the cylinder surfaces, asymmetric material transfer and the generation of wear debris are found in this case. For the b = 0.5 and 1 nm collision, the evolution of third-body volume can be quantitatively described by a simple geometric overlap model that assumes a sliding-induced phase transformation localized between both asperities. For b = 2 nm, this model underestimates the third-body volume by more than 150 % indicating that plasticity has to be taken into account in simple geometric models of severe DLC/DLC asperity collisions.

Sequence of Stages in the Microstructure Evolution in Copper under Mild Reciprocating Tribological Loading.

Tailoring the surface properties of a material for low friction and little wear has long been a goal of tribological research. Since the microstructure of the material under the contact strongly influences tribological performance, the ability to control this microstructure is thereby of key importance. However, there is a significant lack of knowledge about the elementary mechanisms of microstructure evolution under tribological load. To cover different stages of this microstructure evolution, high-purity copper was investigated after increasing numbers of sliding cycles of a sapphire sphere in reciprocating motion. Scanning electron and focused ion beam (FIB) microscopy were applied to monitor the microstructure changes. A thin tribologically deformed layer which grew from tens of nanometers to several micrometers with increasing number of cycles was observed in cross-sections. By analyzing dislocation structures and local orientation changes in the cross-sectional areas, dislocation activity, the occurrence of a distinct dislocation trace line, and the emergence of new subgrain boundaries could be observed at different depths. These results strongly suggest that dislocation self-organization is a key elementary mechanism for the microstructure evolution under a tribological load. The distinct elementary processes at different stages of sliding identified here will be essential for the future modeling of the microstructure evolution in tribological contacts.

Tailored Buckling Microlattices as Reusable Light-Weight Shock Absorbers.

Structures and materials absorbing mechanical (shock) energy commonly exploit either viscoelasticity or destructive modifications. Based on a class of uniaxial light-weight geometrically nonlinear mechanical microlattices and using buckling of inner elements, either a sequence of snap-ins followed by irreversible hysteretic - yet repeatable - self-recovery or multistability is achieved, enabling programmable behavior. Proof-of-principle experiments on three-dimensional polymer microstructures are presented.

Hydrogenated vacancies lock dislocations in aluminium.

Due to its high diffusivity, hydrogen is often considered a weak inhibitor or even a promoter of dislocation movements in metals and alloys. By quantitative mechanical tests in an environmental transmission electron microscope, here we demonstrate that after exposing aluminium to hydrogen, mobile dislocations can lose mobility, with activating stress more than doubled. On degassing, the locked dislocations can be reactivated under cyclic loading to move in a stick-slip manner. However, relocking the dislocations thereafter requires a surprisingly long waiting time of ∼103 s, much longer than that expected from hydrogen interstitial diffusion. Both the observed slow relocking and strong locking strength can be attributed to superabundant hydrogenated vacancies, verified by our atomistic calculations. Vacancies therefore could be a key plastic flow localization agent as well as damage agent in hydrogen environment.