Sliding friction of a pillar array interface: part I.

Biology is replete with examples, at length scales ranging from the molecular (ligand-receptor binding) to the mesoscopic scale (wing arresting structures on dragonflies) where shape-complementary surfaces are used to control interfacial mechanical properties such as adhesion, friction, and contact compliance. Related bio-inspired and biomimetic structures have been used to achieve unique interfacial properties such as friction and adhesion enhancement, directional and switchable properties. The ability to tune friction by altering surface structures offers advantages in various fields, such as soft robotics and tire manufacturing. Here, we present a study of friction between polydimethylsiloxane (PDMS) samples with surfaces patterned with pillar-arrays. When brought in contact with each other the two samples spontaneously produce a Moiré pattern that can also be represented as an array of interfacial dislocations that depends on interfacial misorientation and lattice spacing. Misorientation alone produces an array of screw dislocations, while lattice mismatch alone produces an array of edge dislocations. Relative sliding motion is accompanied by interfacial glide of these patterns. The frictional force resisting dislocation glide arises from periodic single pillar-pillar contact and sliding. We study the behavior of pillar-pillar contact with larger (millimeter scale) pillar samples. Inter-pillar interaction measurements are combined with a geometric model for relative sliding to calculate frictional stress that is in good agreement with experiments.

Sliding friction of a pillar array interface: part II, contact mechanics of single pillar pairs.

Insects and small animals often utilize structured surfaces to create friction during their movements. These surfaces typically consist of pillar-like fibrils that interact with a counter surface. Understanding the mechanical interaction between such surfaces is crucial for designing structured surfaces for engineering applications. In the first part of our study, we examined friction between poly(dimethylsiloxane) (PDMS) samples with surfaces patterned with pillar-arrays. We observed that sliding between these surfaces occurs through the interfacial glide of dislocation structures. The frictional force that resists this dislocation glide is a result of periodic single pillar-pillar contact and sliding. Hence, comprehending the intricate interaction between individual pillar contacts is a fundamental prerequisite for accurately modeling the friction behavior of the pillar array. In this second part of the study, we thoroughly investigated the contact interaction between two pillars located on opposite sides of an interface, with different lateral and vertical offsets. We conducted experiments using PDMS pillars to measure both the reaction shear and normal forces. Contact interaction between pillars was then studied using finite element (FE) simulations with the Coulomb friction model, which yielded results that aligned well with the experimental data. Our result offers a fundamental solution for comprehending how fibrillar surfaces contact and interact during sliding, which has broad applications in both natural and artificial surfaces.

How the geometry of patterned surfaces affects the thickness distribution of the oxidized silica layer on polydimethylsiloxane (PDMS) after ultraviolet/ozone treatment.

It is well established that a thin silica-like surface layer is formed when a cross-linked PDMS structure is subjected to ultraviolet/ozone treatment. Due to surface geometry, especially near the corners, this silica-like surface layer has non-uniform thickness, which can impact many mechanical properties, including adhesion and fracture strength. Here we use a simple analytic model based on diffusion of reactive species to predict the thickness of the oxidized surface layer near the corners. We demonstrate that these corner solutions can be patched together to determine the thickness of the oxidized layer in complex geometries.

Slicing of a soft solid.

Cutting of soft materials is a complex problem, which is still not well understood at the fundamental level, especially for soft materials. The cutting process we consider is slicing, which starts with indentation, followed by sliding of a knife on the material to be cut. Here, we describe cutting experiments on PDMS elastomers with three different moduli. Our experiments reveal typical stages of this cutting process, starting with indentation and ending at steady state cutting. The process starts with a pre-cutting phase in which the blade does not slip grossly relative to the solid to be cut, and deformation is mostly elastic. Slip of the blade initiates suddenly and is often accompanied by initiation of cutting. Cutting is relatively smooth in the next stage, which requires a continuous increase in shear force. For soft PDMS, this smooth cutting stage is followed by one in which folds or creases form on the cutting surface. The corresponding shear force response is no longer smooth as "steady" sliding occurs in a stick-slip fashion with oscillatory forces. The average shear force reaches a plateau and no longer increases with shear displacement. Experimental observations of the various cutting stages are interpreted quantitatively.

The transition from Elasto-Hydrodynamic to Mixed Regimes in Lubricated Friction of Soft Solid Surfaces.

Lubricated contacts in soft materials are common in various engineering and natural settings, such as tires, haptic applications, contact lenses, and the fabrication of soft electronic devices. Two major regimes are elasto-hydrodynamic lubrication (EHL), in which solid surfaces are fully separated by a fluid film, and mixed lubrication (ML), in which there is partial solid-to-solid contact. The transition between these regimes governs the minimum sliding friction achievable and is thus very important. Generally, the transition from EHL to ML regimes is believed to occur when the thickness of the lubricant layer is comparable with the amplitude of surface roughness. Here, it is reported that in lubricated sliding experiments on smooth, soft, poly(dimethylsiloxane) substrates, the transition can occur when the thickness of the liquid layer is much larger than the height of the asperities. Direct visualization of the "contact" region shows that the transition corresponds to the formation of wave-like surface wrinkles at the leading contact edge and associated instabilities at the trailing contact edge, which are believed to trigger the transition to the mixed regime. These results change the understanding of what governs the important EHL-ML transition in the lubricated sliding of soft solids.

Penetration of Cell Surface Glycocalyx by Enveloped Viruses Is Aided by Weak Multivalent Adhesive Interaction.

Viral infection usually begins with adhesion between the viral particle and viral receptors displayed on the cell membrane. The exterior surface of the cell membrane is typically coated with a brush-like layer of molecules, the glycocalyx, that the viruses need to penetrate. Although there is extensive literature on the biomechanics of virus-cell adhesion, much of it is based on continuum-level models that do not address the question of how virus/cell-membrane adhesion occurs through the glycocalyx. In this work, we present a simulation study of the penetration mechanism. Using a coarse-grained molecular model, we study the force-driven and diffusive penetration of a brush-like glycocalyx by viral particles. For force-driven penetration, we find that viral particles smaller than the spacing of molecules in the brush reach the membrane surface readily. For a given maximum force, viral particles larger than the minimum spacing of brush molecules arrest at some distance from the membrane, governed by the balance of elastic and applied forces. For the diffusive case, we find that weak but multivalent attraction between the glycocalyx molecules and the virus effectively leads to its engulfment by the glycocalyx. Our finding provides potential guidance for developing glycocalyx-targeting drugs and therapies by understanding how virus-cell adhesion works.

Fast, strong, and reversible adhesives with dynamic covalent bonds for potential use in wound dressing.

Adhesives typically fall into two categories: those that have high but irreversible adhesion strength due to the formation of covalent bonds at the interface and are slow to deploy, and others that are fast to deploy and the adhesion is reversible but weak in strength due to formation of noncovalent bonds. Synergizing the advantages from both categories remains challenging but pivotal for the development of the next generation of wound dressing adhesives. Here, we report a fast and reversible adhesive consisting of dynamic boronic ester covalent bonds, formed between poly(vinyl alcohol) (PVA) and boric acid (BA) for potential use as a wound dressing adhesive. Mechanical testing shows that the adhesive film has strength in shear of 61 N/cm2 and transcutaneous adhesive strength of 511 N/cm2, generated within 2 min of application. Yet the film can be effortlessly debonded when exposed to excess water. The mechanical properties of PVA/BA adhesives are tunable by varying the cross-linking density. Within seconds of activation by water, the surface boronic ester bonds in the PVA/BA film undergo fast debonding and instant softening, leading to conformal contact with the adherends and reformation of the boronic ester bonds at the interface. Meanwhile, the bulk film remains dehydrated to offer efficient load transmission, which is important to achieve strong adhesion without delamination at the interface. Whether the substrate surface is smooth (e.g., glass) or rough (e.g., hairy mouse skin), PVA/BA adhesives demonstrate superior adhesion compared to the most widely used topical skin adhesive in clinical medicine, Dermabond.

Detection of ovarian cancer via the spectral fingerprinting of quantum-defect-modified carbon nanotubes in serum by machine learning.

Serum biomarkers are often insufficiently sensitive or specific to facilitate cancer screening or diagnostic testing. In ovarian cancer, the few established serum biomarkers are highly specific, yet insufficiently sensitive to detect early-stage disease and to impact the mortality rates of patients with this cancer. Here we show that a 'disease fingerprint' acquired via machine learning from the spectra of near-infrared fluorescence emissions of an array of carbon nanotubes functionalized with quantum defects detects high-grade serous ovarian carcinoma in serum samples from symptomatic individuals with 87% sensitivity at 98% specificity (compared with 84% sensitivity at 98% specificity for the current best clinical screening test, which uses measurements of cancer antigen 125 and transvaginal ultrasonography). We used 269 serum samples to train and validate several machine-learning classifiers for the discrimination of patients with ovarian cancer from those with other diseases and from healthy individuals. The predictive values of the best classifier could not be attained via known protein biomarkers, suggesting that the array of nanotube sensors responds to unidentified serum biomarkers.

Machine Learning-Guided Systematic Search of DNA Sequences for Sorting Carbon Nanotubes.

The prerequisite of utilizing DNA in sequence-dependent applications is to search specific sequences. Developing a strategy for efficient DNA sequence screening represents a grand challenge due to the countless possibilities of sequence combination. Herein, relying on sequence-dependent recognition between DNA and single-wall carbon nanotubes (SWCNTs), we demonstrate a method for systematic search of DNA sequences for sorting single-chirality SWCNTs. Different from previously documented empirical search, which has a low efficiency and accuracy, our approach combines machine learning and experimental investigation. The number of resolving sequences and the success rate of finding them are improved from ∼102 to ∼103 and from ∼10% to >90%, respectively. Moreover, the resolving sequence patterns determined from 5-mer and 6-mer short sequences can be extended to sequence search in longer DNA subspaces.

Lubricated soft normal elastic contact of a sphere: a new numerical method and experiment.

An important problem in lubrication is the squeezing of a thin liquid film between a rigid sphere and an elastic substrate under normal contact. Numerical solution of this problem typically uses iteration techniques. A difficulty with iteration schemes is that convergence becomes increasingly difficult under increasingly heavy loads. Here we devise a numerical scheme that does not involve iteration. Instead, a linear problem is solved at every time step. The scheme is fully automatic, stable and efficient. We illustrate this technique by solving a relaxation test in which a rigid spherical indenter is brought rapidly into normal contact with a thick elastic substrate lubricated by a liquid film. The sphere is then fixed in position as the pressure relaxes. We also carried out relaxation experiments on a lubricated soft PDMS (polydimethysiloxane) substrate under different conditions. These experiments are in excellent agreement with the numerical solution.

Surface Tension and the Strain-Dependent Topography of Soft Solids.

When stretched in one direction, most solids shrink in the transverse directions. In soft silicone gels, however, we observe that small-scale topographical features grow upon stretching. A quantitative analysis of the topography shows that this counterintuitive response is nearly linear, allowing us to tackle it through a small-strain analysis. We find that the surprising increase of small-scale topography with stretch is due to a delicate interplay of the bulk and surface responses to strain. Specifically, we find that surface tension changes as the material is deformed. This response is expected on general grounds for solid materials, but challenges the standard description of gel and elastomer surfaces.

A perception-based nanosensor platform to detect cancer biomarkers.

Conventional molecular recognition elements, such as antibodies, present issues for developing biomolecular assays for use in certain technologies, such as implantable devices. Additionally, antibody development and use, especially for highly multiplexed applications, can be slow and costly. We developed a perception-based platform based on an optical nanosensor array that leverages machine learning algorithms to detect multiple protein biomarkers in biofluids. We demonstrated this platform in gynecologic cancers, often diagnosed at advanced stages, leading to low survival rates. We investigated the detection of protein biomarkers in uterine lavage samples, which are enriched with certain cancer markers compared to blood. We found that the method enables the simultaneous detection of multiple biomarkers in patient samples, with F1-scores of ~0.95 in uterine lavage samples from patients with cancer. This work demonstrates the potential of perception-based systems for the development of multiplexed sensors of disease biomarkers without the need for specific molecular recognition elements.

A surface flattening method for characterizing the surface stress, drained Poisson's ratio and diffusivity of poroelastic gels.

When a poroelastic gel is released from a patterned mold, surface stress drives deformation and solvent migration in the gel and flattens its surface profile in a time-dependent manner. Specifically, the gel behaves like an incompressible solid immediately after removal from the mold, and becomes compressible as the solvent is able to squeeze out of the polymer network. In this work, we use the finite element method (FEM) to simulate this transient surface flattening process. We assume that the surface stress is isotropic and constant, the polymer network is linearly elastic and isotropic, and that solvent flow obeys Darcy's law. The short-time and long-time surface profiles can be used to determine the surface stress and drained Poisson's ratio of the gel. Our analysis shows that the drained Poisson's ratio and the diffusivity of the gel can be obtained using interferometry and high-speed video microscopy, without mechanical measurement.

Meso-scale dislocations and friction of shape-complementary soft interfaces.

The interface between two surfaces patterned with complementary shapes such as arrays of ridge-channel structures or pillars accommodates relative misorientation and lattice mismatch by spontaneous production of dislocation arrays. Here, we show that the relative sliding of such an interface is accomplished by dislocation glide on the interfacial plane. An exception is the singular case where the lattices are perfectly matched across the sample dimension, in which case sliding is accompanied by motion of edge-nucleated defects. These are meso-scale analogues of molecular sliding friction mechanisms between crystalline interfaces. The dislocations, in addition to the long-range elastic energy associated with their Burgers vectors, also cause significant out-of-plane dilation, which props open the interface locally. For this reason, the sliding friction is strongly pressure dependent; it also depends on the relative orientation of the patterns. Sliding friction can be strongly enhanced compared with a control, showing that shape-complementary interfaces can be engineered for strongly enhanced pressure- and orientation-dependent frictional properties in soft solids.

Length of mucin-like domains enhances cell-Ebola virus adhesion by increasing binding probability.

The Ebola virus (EBOV) hijacks normal physiological processes by apoptotic mimicry to be taken up by the cell it infects. The initial adhesion of the virus to the cell is based on the interaction between T cell immunoglobulin and mucin domain protein, TIM, on the cell surface and phosphatidylserine (PS) on the viral outer surface. Therefore, it is important to understand the interaction between EBOV and PS and TIM, with selective blocking of the interaction as a potential therapy. Recent experimental studies have shown that for TIM-dependent EBOV entry, a mucin-like domain with a length of at least 120 amino acids is required, possibly because of the increase of area of the PS-coated surface sampled. We examine this hypothesis by modeling the process of TIM-PS adhesion using a coarse-grained molecular model. We find that the strength of individual bound PS-TIM pairs is essentially independent of TIM length. TIMs with longer mucin-like domains collectively have higher average binding strengths because of an increase in the probability of binding between EBOV and TIM proteins. Similarly, we find that for larger persistence length (less flexible), the average binding force decreases, again because of a reduction in the probability of binding.

How surface stress transforms surface profiles and adhesion of rough elastic bodies.

The surface of soft solids carries a surface stress that tends to flatten surface profiles. For example, surface features on a soft solid, fabricated by moulding against a stiff-patterned substrate, tend to flatten upon removal from the mould. In this work, we derive a transfer function in an explicit form that, given any initial surface profile, shows how to compute the shape of the corresponding flattened profile. We provide analytical results for several applications including flattening of one-dimensional and two-dimensional periodic structures, qualitative changes to the surface roughness spectrum, and how that strongly influences adhesion.

Modeling of surface mechanical behaviors of soft elastic solids: theory and examples.

Surfaces of soft solids can have significant surface stress, extensional modulus and bending stiffness. Previous theoretical studies have usually examined cases in which both the surface stress and bending stiffness are constant, assuming small deformation. In this work we consider a general formulation in which the surface can support large deformation and carry both surface stresses and surface bending moments. We demonstrate that the large deformation theory can be reduced to the classical linear theory (Shuttleworth equation). We obtain exact solutions for problems of an inflated cylindrical shell and bending of a plate with a finite thickness. Our analysis illustrates the different manners in which surface stiffening and surface bending stabilize these structures. We discuss how the complex surface constitutive behaviors affect the stress field of the bulk. Our calculation provides insights into effects of strain-dependent surface stress and surface bending in the large deformation regime, and can be used as a model to implement surface finite elements to study large deformation of complex structures.

Lubricated steady sliding of a rigid sphere on a soft elastic substrate: hydrodynamic friction in the Hertz limit.

Lubricated sliding on soft elastic substrates occurs in a variety of natural and technological settings. It very often occurs in the iso-viscous elasto-hydrodynamic lubrication (EHL) regime (e.g., soft solid, low pressure). In this regime, for sliding of a smooth sphere on a soft solid, a "Hertz-like" effective contact region forms. Much of the fluid is squeezed out of the contact region although enough is retained to keep the solid surfaces fully separated. This is accompanied by complex deformation of the soft solid. The behavior of such soft lubricated contacts is controlled by a single dimensionless parameter 1/ß that can be interpreted as a normalized sliding velocity. Solving this fundamental soft-lubrication problem poses significant computational difficulty for large ß, which is the limit relevant for soft solids. As a consequence, little is known about the structure of the flow field under soft lubrication in the intake and outlet regions. Here we present a new solution of this soft lubrication problem focusing on the "Hertz" limit. We develop a formulation in polar coordinates that handles difficult computational issues much better than previous methods. We study how hydrodynamic pressure, film thickness and hydrodynamic friction vary with ß. Scaling laws for these relationships are given in closed form for a range of ß not previously accessible theoretically but that is typical in applications. The computational method presented here can be used to study other soft lubrication problems.

Enhancement of elastohydrodynamic friction by elastic hysteresis in a periodic structure.

Lubricated contacts are present in many engineering and biological systems involving soft solids. Typical mechanisms considered for controlling the sliding friction in such lubricated conditions involve bulk material compliance, fluid viscosity, viscoelastic response of the material (hysteretic friction), and breaking of the fluid film where dry contact occurs (adhesive friction). In this work we show that a two-phase periodic structure (TPPS), with a varying modulus across the sliding surface, provides significant enhancement of lubricated sliding friction when the system is in the elastohydrodynamic lubrication (EHL) regime. We propose that the enhanced friction is due to extra energy loss during periodic transitions of the sliding indenter between the compliant and stiff regions during which excess energy is dissipated through the fluid layer. This is a form of elastic hysteresis that provides a novel mechanism for friction enhancement in soft solids under lubricated conditions.