No Arabic abstract
A mechanistic understanding of adhesion in soft materials is critical in the fields of transportation (tires, gaskets, seals), biomaterials, micro-contact printing, and soft robotics. Measurements have long demonstrated that the apparent work of adhesion coming into contact is consistently lower than the intrinsic work of adhesion for the materials, and that there is adhesion hysteresis during separation, commonly explained by viscoelastic dissipation. Still lacking is a quantitative experimentally validated link between adhesion and measured topography. Here, we used in situ measurements of contact size to investigate the adhesion behavior of soft elastic polydimethylsiloxane (PDMS) hemispheres (modulus ranging from 0.7 to 10 MPa) on four different polycrystalline diamond substrates with topography characterized across eight orders of magnitude, including down to the r{A}ngstrom-scale. The results show that the reduction in apparent work of adhesion is equal to the energy required to achieve conformal contact. Further, the energy loss during contact and removal is equal to the product of intrinsic work of adhesion and the true contact area. These findings provide a simple mechanism to quantitatively link the widely-observed adhesion hysteresis to roughness rather than viscoelastic dissipation.
Surface topography strongly modifies adhesion of hard-material contacts, yet roughness of real surfaces typically exists over many length scales. This investigation aims to determine which scales of topography have the strongest effect on macroscopic adhesion. Adhesion measurements were performed on technology-relevant diamond coatings of varying roughness using spherical ruby probes that are large enough ($0.5$-mm-diameter) to sample all length scales of topography. For each material, more than $2000$ measurements of pull-off force were performed in order to investigate the magnitude and statistical distribution of adhesion. Using sphere-contact models, the roughness-dependent effective values of work of adhesion were measured, ranging from $0.08$ to $7.15$ mJ/m$^2$ across the four surfaces. The data was more accurately fit using numerical analysis, where an interaction potential was integrated over the AFM-measured topography of all contacting surfaces. These calculations revealed that consideration of nanometer-scale plasticity in the materials was crucial for a good quantitative fit of the measurements, and the presence of such plasticity was confirmed with AFM measurements of the probe after testing. This analysis enabled the extraction of geometry-independent material parameters; the intrinsic work of adhesion between ruby and diamond was determined to be $46.3$ mJ/m$^2$. The range of adhesion was $5.6$ nm, which is longer than is typically assumed for atomic interactions, but is in agreement with other recent investigations. Finally, the numerical analysis was repeated for the same surfaces but this time with different length-scales of roughness included or filtered out. The results demonstrate a critical band of length-scales between $43$ nm and $1.8$ nm in lateral size that has the strongest effect on the total adhesive force for these hard, rough contacts.
Activity and self-generated motion are fundamental features observed in many living and non-living systems. Given that inter-particle adhesive forces are known to regulate particle dynamics, we investigate how adhesion strength controls the boundary growth and roughness in an active particle aggregate. Using particle based simulations incorporating both activity (birth, death and growth) and systematic physical interactions (elasticity and adhesion), we establish that inter-particle adhesion strength ($f^{ad}$) controls the surface roughness of a densely packed three-dimensional(3D) active particle aggregate expanding into a highly viscous medium. We discover that the surface roughness of a 3D active particle aggregate increases in proportion to the inter-particle adhesion strength, $f^{ad}$. We show that asymmetry in the radial and tangential active particle mean squared displacement (MSD) suppresses 3D surface roughness at lower adhesion strengths. By analyzing the statistical properties of particle displacements at the aggregate periphery, we determine that the 3D surface roughness is driven by the movement of active particle towards the core at high inter-particle adhesion strengths. Our results elucidate the physics controlling the expansion of adhesive 3D active particle collectives into a highly viscous medium, with implications into understanding stochastic interface growth in active matter systems characterized by self generated particle flux.
The motion of soft-glassy materials (SGM) in a confined geometry is strongly impacted by surface roughness. However, the effect of the spatial distribution of the roughness remains poorly understood from a more quantitative viewpoint. Here we present a comprehensive study of concentrated emulsions flowing in microfluidic channels, one wall of which is patterned with micron-size equally spaced grooves oriented perpendicularly to the flow direction. We show that roughness-induced fluidization can be quantitatively tailored by systematically changing both the width and separation of the grooves. We find that a simple scaling law describes such fluidization as a function of the density of grooves, suggesting common scenarios for droplet trapping and release. Numerical simulations confirm these views and are used to elucidate the relation between fluidization and the rate of plastic rearrangements.
We study the influence of surface roughness on the adhesion of elastic solids. Most real surfaces have roughness on many different length scales, and this fact is taken into account in our analysis. We consider in detail the case when the surface roughness can be described as a self affine fractal, and show that when the fractal dimension D_f >2.5, the adhesion force may vanish, or be at least strongly reduced. We consider the block-substrate pull-off force as a function of roughness, and find a partial detachment transition preceding a full detachment one. The theory is in good qualitative agreement with experimental data.
Surface stress and surface energy are two fundamental parameters that determine the surface properties of any material. While it is commonly believed that the surface stress and surface energy of liquids are identical, the relationship between the two parameters in soft polymeric gels remains debatable. In this work, we measured the surface stress and surface energy of soft silicone gels with varying crosslinking densities in soft wetting experiments. Above a critical crosslink density, $k_0$, the surface stress is found to increase significantly with crosslinking density while the surface energy, by contrast, remains unchanged. In this regime, we can estimate a non-zero surface elastic modulus that also increases with the ratio of crosslinkers. By comparing the surface mechanics of the soft gels to their bulk rheology, the surface properties near the critical density $k_0$ are found to be closely related to the underlying percolation transition of the polymer networks.