A simple approach to produce hydrophobic biobased coatings using methylcellulose and organosolv lignin.

Substituting plastics with circular and sustainable alternatives has increasingly become a priority. Protective coatings, crucial components in numerous industries, are now in demand for biodegradable options to replace their plastic-based counterparts. Being one of nature's most abundant components, lignin remains underutilized, and this study focuses on investigating its potential for the production of biobased coatings. The method used here involved formulating coating suspensions by mixing methylcellulose and organosolv lignin powders and adding water to the mixture. Glass wafers were coated with the formulated suspensions using spin-coating. The morphology of the coated surfaces was assessed using optical and scanning electron microscopy. In addition, the wettability of the surfaces was examined through water contact angle experiments, and a numerical model was introduced to predict the water contact angle evolution over time. The results revealed that the sample coated with a 2.5 wt% lignin suspension exhibited the highest initial contact angle (114°), with a decreasing trend as the lignin fraction increases. Moreover, coatings with 3.5 wt% lignin and above exhibited lower surface coverage due to lignin particle aggregation and surface defects. By approximating the water droplet on the surface as a spherical cap, the introduced numerical model successfully predicted the time-dependent evolution of the water contact angle by showing strong alignment with experimental results. Taken altogether, we have showcased here a method for modifying coating properties-in a practical sense from water-absorbent to splash-proof-using readily available forest-based materials. This advancement is paving the way for sustainable protective packaging, aiming to replace styrofoam in the electronics and food industries.

Impurity-induced nematic-isotropic transition of liquid crystals.

Complex fluids made of liquid crystals (LCs) and small molecules, surfactants, nanoparticles or 1D/2D nanomaterials show novel and interesting features, making them suitable materials for various applications starting from optoelectronics to biosensing. While these additives (impurities) introduce new features in the complex fluids, they may also alter the phase transition behaviour of LCs depending on the physiochemical properties of the added impurity. This article reports on the phase transition of 4-cyano-4'-alkylbiphenyl (nCB) LCs in the presence of an associative impurity, i.e., water and a non-associative impurity, i.e., hexane employing computational methods and experiments. In particular, all-atom (AA) simulations and coarse-grained (CG) models were designed for two complex systems, i.e., 6CB + water and 6CB + hexane and corresponding spectrophotometry experiments were performed using a homologous LC, i.e., 5CB. Results from the simulations and experiments elucidate that the phase transition of LCs depends on the mixing/demixing phenomenon of the impurity in the LC. While associative liquids like water which do not mix with LCs do not influence the nematic-to-isotropic phase transition of LCs, hexane, being a non-associative liquid, mixes well with LCs and induces a sharp impurity-induced nematic-to-isotropic phase transition. Upon application of both AA and CG simulations, we could reach the conclusion that the mixing/demixing phenomenon in an LC + impurity system influences the entropy of the system and hence the observed phase transitions are entropy-driven.

Crossover from mean-field compression to collective phenomena in low-density foam-formed fiber material.

We study the compression of low-weight foam-formed materials made out of wood fibers. Initially the stress-strain behavior follows mean-field like response, related to the buckling of fiber segments as dictated by the random three-dimensional geometry. Our Acoustic Emission (AE) measurements correlate with the predicted number of segment bucklings for increasing strain. However, the experiments reveal a transition to collective phenomena as the strain increases sufficiently. This is also seen in the gradual failure of the theory to account for the stress-strain curves. The collective avalanches exhibit scale-free features both as regards the AE energy distribution and the AE waiting time distributions with both exponents having values close to 2. In cyclic compression tests, significant increases in the accumulated acoustic energy are found only when the compression exceeds the displacement of the previous cycle, which further confirms other sources of acoustic events than fiber bending.

Bursts of activity in collective cell migration.

Dense monolayers of living cells display intriguing relaxation dynamics, reminiscent of soft and glassy materials close to the jamming transition, and migrate collectively when space is available, as in wound healing or in cancer invasion. Here we show that collective cell migration occurs in bursts that are similar to those recorded in the propagation of cracks, fluid fronts in porous media, and ferromagnetic domain walls. In analogy with these systems, the distribution of activity bursts displays scaling laws that are universal in different cell types and for cells moving on different substrates. The main features of the invasion dynamics are quantitatively captured by a model of interacting active particles moving in a disordered landscape. Our results illustrate that collective motion of living cells is analogous to the corresponding dynamics in driven, but inanimate, systems.

Nanoscale liquid crystal lubrication controlled by surface structure and film composition.

Liquid crystals have emerged as potential candidates for next-generation lubricants due to their tendency to exhibit long-range ordering. Here, we construct a full atomistic model of 4-cyano-4-hexylbiphenyl (6CB) nematic liquid crystal lubricants mixed with hexane and confined by mica surfaces. We explore the effect of the surface structure of mica, as well as lubricant composition and thickness, on the nanoscale friction in the system. Our results demonstrate the key role of the structure of the mica surfaces, specifically the positions of potassium (K+) ions, in determining the nature of sliding friction with monolayer lubricants, including the presence or absence of stick-slip dynamics. With the commensurate setup of confining surfaces, when the grooves created between the periodic K+ ions are parallel to the sliding direction we observe a lower friction force as compared to the perpendicular situation. Random positions of ions exhibit even smaller friction forces with respect to the previous two cases. For thicker lubrication layers the surface structure becomes less important and we observe a good agreement with the experimental data on bulk viscosity of 6CB and the additive hexane. In case of thicker lubrication layers, friction may still be controlled by tuning the relative concentrations of 6CB and hexane in the mixture.

Excitation Spectra in Crystal Plasticity.

Plastically deforming crystals exhibit scale-free fluctuations that are similar to those observed in driven disordered elastic systems close to depinning, but the nature of the yielding critical point is still debated. Here, we study the marginal stability of ensembles of dislocations and compute their excitation spectrum in two and three dimensions. Our results show the presence of a singularity in the distribution of excitation stresses, i.e., the stress needed to make a localized region unstable, that is remarkably similar to the one measured in amorphous plasticity and spin glasses. These results allow us to understand recent observations of extended criticality in bursty crystal plasticity and explain how they originate from the presence of a pseudogap in the excitation spectrum.

Interevent Correlations from Avalanches Hiding Below the Detection Threshold.

Numerous systems ranging from deformation of materials to earthquakes exhibit bursty dynamics, which consist of a sequence of events with a broad event size distribution. Very often these events are observed to be temporally correlated or clustered, evidenced by power-law-distributed waiting times separating two consecutive activity bursts. We show how such interevent correlations arise simply because of a finite detection threshold, created by the limited sensitivity of the measurement apparatus, or used to subtract background activity or noise from the activity signal. Data from crack-propagation experiments and numerical simulations of a nonequilibrium crack-line model demonstrate how thresholding leads to correlated bursts of activity by separating the avalanche events into subavalanches. The resulting temporal subavalanche correlations are well described by our general scaling description of thresholding-induced correlations in crackling noise.

Avalanches in Wood Compression.

Wood is a multiscale material exhibiting a complex viscoplastic response. We study avalanches in small wood samples in compression. "Woodquakes" measured by acoustic emission are surprisingly similar to earthquakes and crackling noise in rocks and laboratory tests on brittle materials. Both the distributions of event energies and of waiting (silent) times follow power laws. The stress-strain response exhibits clear signatures of localization of deformation to "weak spots" or softwood layers, as identified using digital image correlation. Even though material structure-dependent localization takes place, the avalanche behavior remains scale-free.

Stick-slip control in nanoscale boundary lubrication by surface wettability.

We study the effect of atomic-scale surface-lubricant interactions on nanoscale boundary-lubricated friction by considering two example surfaces-hydrophilic mica and hydrophobic graphene-confining thin layers of water in molecular dynamics simulations. We observe stick-slip dynamics for thin water films confined by mica sheets, involving periodic breaking-reforming transitions of atomic-scale capillary water bridges formed around the potassium ions of mica. However, only smooth sliding without stick-slip events is observed for water confined by graphene, as well as for thicker water layers confined by mica. Thus, our results illustrate how atomic-scale details affect the wettability of the confining surfaces and consequently control the presence or absence of stick-slip dynamics in nanoscale friction.

Apparent wall slip in non-Brownian hard-sphere suspensions.

We analyze apparent wall slip, the reduction of particle concentration near the wall, in hard-sphere suspensions at concentrations well below the jamming limit utilizing a continuum level diffusion model. The approach extends a constitutive equation proposed earlier with two additional potentials describing the effects of gravitation and wall-particle repulsion. We find that although both mechanisms are shear independent by nature, due to the shear-rate-dependent counter-balancing particle migration fluxes, the resulting net effect is non-linearly shear dependent, causing larger slip at small shear rates. In effect, this shows up in the classically measured flow curves as a mild shear thickening regime at the transition from small to intermediate shear rates.

Avalanches in 2D dislocation systems: plastic yielding is not depinning.

We study the properties of strain bursts (dislocation avalanches) occurring in two-dimensional discrete dislocation dynamics models under quasistatic stress-controlled loading. Contrary to previous suggestions, the avalanche statistics differ fundamentally from predictions obtained for the depinning of elastic manifolds in quenched random media. Instead, we find an exponent τ=1 of the power-law distribution of slip or released energy, with a cutoff that increases exponentially with the applied stress and diverges with system size at all stresses. These observations demonstrate that the avalanche dynamics of 2D dislocation systems is scale-free at every applied stress and, therefore, cannot be envisaged in terms of critical behavior associated with a depinning transition.

Rheology dynamics of aggregating colloidal suspensions.

We study a colloidal model based on population balances in the context of complex fluid rheology. Two typical particle microstructure kinetics, orthokinetic, collisions due to shear, and perikinetic, collisions due to Brownian motion, are found to appear at continuum as different flow behaviors - those having monotonic and non-monotonic flow curves, respectively. Solving the colloidal model together with the 1D Stokes equation for laminar, incompressible flow with Couette boundary conditions, allows bridging the gap between the rheological experiments and the microstructural modeling. The analysis of such a model reveals that orthokinetic particle suspensions have a uniquely defined, continuous steady state shear profile, whereas suspensions in which also perikinetic collisions are present, the steady state can be shear banded and non-unique. Thus, the shear banded configurations at a steady state are found to depend on the initial conditions and the collision kinetics of the system. At high shear rates all the studied cases show continuous shear profiles.

Dynamic hysteresis in cyclic deformation of crystalline solids.

The hysteresis or internal friction in the deformation of crystalline solids stressed cyclically is studied from the viewpoint of collective dislocation dynamics. Stress-controlled simulations of a dislocation dynamics model at various loading frequencies and amplitudes are performed to study the stress-strain rate hysteresis. The hysteresis loop areas exhibit a maximum at a characteristic frequency and a power law frequency dependence in the low frequency limit, with the power law exponent exhibiting two regimes, corresponding to the jammed and the yielding or moving phases of the system, respectively. The first of these phases of the system exhibits nontrivial critical-like viscoelastic dynamics, crossing over to intermittent viscoplastic deformation for higher stress amplitudes.

Fracture strength of disordered media: universality, interactions, and tail asymptotics.

We study the asymptotic properties of fracture strength distributions of disordered elastic media by a combination of renormalization group, extreme value theory, and numerical simulation. We investigate the validity of the "weakest-link hypothesis" in the presence of realistic long-ranged interactions in the random fuse model. Numerical simulations indicate that the fracture strength is well-described by the Duxbury-Leath-Beale (DLB) distribution which is shown to flow asymptotically to the Gumbel distribution. We explore the relation between the extreme value distributions and the DLB-type asymptotic distributions and show that the universal extreme value forms may not be appropriate to describe the nonuniversal low-strength tail.

Modelling aerosol-based exposure to SARS-CoV-2 by an agent based Monte Carlo method: Risk estimates in a shop and bar.

Present day risk assessment on the spreading of airborne viruses is often based on the classical Wells-Riley model assuming immediate mixing of the aerosol into the studied environment. Here, we improve on this approach and the underlying assumptions by modeling the space-time dependency of the aerosol concentration via a transport equation with a dynamic source term introduced by the infected individual(s). In the present agent-based methodology, we study the viral aerosol inhalation exposure risk in two scenarios including a low/high risk scenario of a "supermarket"/"bar". The model takes into account typical behavioral patterns for determining the rules of motion for the agents. We solve a diffusion model for aerosol concentration in the prescribed environments in order to account for local exposure to aerosol inhalation. We assess the infection risk using the Wells-Riley model formula using a space-time dependent aerosol concentration. The results are compared against the classical Wells-Riley model. The results indicate features that explain individual cases of high risk with repeated sampling of a heterogeneous environment occupied by non-equilibrium concentration clouds. An example is the relative frequency of cases that might be called superspreading events depending on the model parameters. A simple interpretation is that averages of infection risk are often misleading. They also point out and explain the qualitative and quantitative difference between the two cases-shopping is typically safer for a single individual person.

Scalable method for bio-based solid foams that mimic wood.

Mimicking natural structures allows the exploitation of proven design concepts for advanced material solutions. Here, our inspiration comes from the anisotropic closed cell structure of wood. The bubbles in our fiber reinforced foam are elongated using temperature dependent viscosity of methylcellulose and constricted drying. The oriented structures lead to high yield stress in the primary direction; 64 times larger than compared to the cross direction. The closed cells of the foam also result in excellent thermal insulation. The proposed novel foam manufacturing process is trivial to up-scale from the laboratory trial scale towards production volumes on industrial scales.

Dynamical correlations near dislocation jamming.

Dislocation assemblies exhibit a jamming or yielding transition at a critical external shear stress value σ=σ{c}. Here we study the heterogeneous and collective nature of dislocation dynamics within a crystal plasticity model close to σ{c}, by considering the first-passage properties of the dislocation dynamics. As the transition is approached in the moving phase, the first-passage time distribution exhibits scaling, and a related peak dynamical susceptibility χ{4}{*} diverges as χ{4}{*}∼(σ-σ{c}){-α}, with α≈1.1. We relate this scaling to an avalanche description of the dynamics. While the static structural correlations are found to be independent of the external stress, we identify a diverging dynamical correlation length ξ{y} in the direction perpendicular to the dislocation glide motion.

Fluctuations and scaling in creep deformation.

The spatial fluctuations of deformation are studied in the creep in Andrade's power law and the logarithmic phases, using paper samples. Measurements by the digital image correlation technique show that the relative strength of the strain rate fluctuations increases with time, in both creep regimes. In the Andrade creep phase characterized by a power-law decay of the strain rate ϵt∼t(-θ), with θ≈0.7, the fluctuations obey Δϵt∼t(-γ), with γ≈0.5. The local deformation follows a data collapse appropriate for a phase transition. Similar behavior is found in a crystal plasticity model, with a jamming or yielding transition.

From brittle to ductile fracture in disordered materials.

We introduce a lattice model able to describe damage and yielding in heterogeneous materials ranging from brittle to ductile ones. Ductile fracture surfaces, obtained when the system breaks once the strain is completely localized, are shown to correspond to minimum energy surfaces. The similarity of the resulting fracture paths to the limits of brittle fracture or minimum energy surfaces is quantified. The model exhibits a smooth transition from brittleness to ductility. The dynamics of yielding exhibits avalanches with a power-law distribution.

Propagating bands of plastic deformation in a metal alloy as critical avalanches.

The plastic deformation of metal alloys localizes in the Portevin-Le Chatelier effect in bands of different types, including propagating, or type "A" bands, usually characterized by their width and a typical propagation velocity. This plastic instability arises from collective dynamics of dislocations interacting with mobile solute atoms, but the resulting sensitivity to the strain rate lacks fundamental understanding. Here, we show, by using high-resolution imaging in tensile deformation experiments of an aluminum alloy, that the band velocities exhibit large fluctuations. Each band produces a velocity signal reminiscent of crackling noise bursts observed in numerous driven avalanching systems from propagating cracks in fracture to the Barkhausen effect in ferromagnets. The statistical features of these velocity bursts including their average shapes and size distributions obey predictions of a simple mean-field model of critical avalanche dynamics. Our results thus reveal a previously unknown paradigm of criticality in the localization of deformation.