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Lorenzo Botto

Publications and source records attributed to Lorenzo Botto.

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Peeling threshold for removal of an adhered elastic sheet by a shear flow

Fluid shear can induce detachment of a thin elastic sheet adhered to a flat substrate. This peeling process is important in a variety of environmental and technological systems. The condition for peeling depends on: the shear rate $\dot{\gamma}$, the fluid viscosity $\eta$, the length of the detached portion of the sheet $L$, the bending rigidity $B$ and the adhesion energy $\Gamma$. What are the laws governing the detachment? We address this question experimentally in the regime of intermediate adhesion, using macroscopic sheets bonded to a substrate and immersed in a shear cell containing a viscous fluid. The experiments indicate a critical shear rate for peeling of the order of $\dot{\gamma} \sim B/(\eta L^3)$. This threshold is, unexpectedly, independent of adhesion. We rationalise this result by applying Griffith's fracture theory to optical measurement data of the shape of the sheet, under conditions of freely moving peeling front or clamped boundary. The results indicate that the large curvature of the sheet for $\dot{\gamma} \sim B/(\eta L^3)$ yields a nearly diverging strain energy release rate at this threshold. This approximate divergence in turn yields a peeling threshold that depends at most weakly on $\Gamma$, confirming a theory that was proposed recently (Salussolia et al., J. Mech. Phys. Solids, 2020, 134). Among other applications, our work provides a quantitative formula that can aid the production at scale of 2D materials such as graphene.

cond-mat.soft

Flapping instability of elastic disks in Stokes flows

Fluid-structure interactions at low Reynolds number can lead to a much richer phenomenology than previously expected. Here, we study the dynamics of a freely suspended, thin elastic disk in a shear flow, where the plane of the disk is initially parallel to the flow plane. Using a combination of experiments and simulations, we demonstrate that beyond a critical flow strength the disk deforms, performing flapping dynamics, in which the disk curves up and down periodically relative to the horizontal shear plane. The bifurcation diagram obtained by simulation reveals several oscillatory solutions, including a wiggling motion that is predicted by a linear stability analysis. The flapping dynamics is shown to be a subcritical instability whose key ingredient is the finite extensibility of the disk. The behavior we observe has implications for emerging investigations on the flow dynamics of sheet-like particles, such as 2D polymers and 2D crystalline materials immersed in viscous fluids.

physics.flu-dyn

Negative intrinsic viscosity in graphene nanoparticle suspensions induced by hydrodynamic slip

The viscosity of nanoparticle suspensions is always expected to increase with particle concentration. However, a growing body of experiments on suspensions of atomically thin nanomaterials such as graphene contradicts this expectation. Some experiments indicate effective suspension viscosity values that fall below that of pure solvent at high shear rates and low solid concentrations, i.e., the intrinsic viscosity is negative. To explain this puzzling phenomenon, we combined molecular dynamics and boundary integral simulations to investigate the shear viscosity of few-nanometer graphene sheets in water at high Péclet numbers (Pe $> 100$). Our results, covering geometric aspect ratios from 4.5 to 12.0, show robustly that the intrinsic viscosity decreases with increasing aspect ratio and becomes negative beyond a threshold aspect ratio $\approx 5.5$. We demonstrate that this anomalous behavior originates from hydrodynamic slip at the liquid-solid interface, which suppresses particle rotation and promotes stable alignment with the flow direction, thereby reducing viscous dissipation relative to dissipation in pure solvent. This slip mechanism holds for both fully 3D disc-like and quasi-2D particle geometries explored in the molecular simulations. As the concentration of graphene particles increases in the dilute regime, the viscosity initially decreases, falling below that of pure water. At higher concentrations, however, particle aggregation becomes significant, leading to a rise in viscosity after a minimum is reached. These findings confirm the occurrence of a negative intrinsic viscosity in a graphene suspension due only to hydrodynamic effects. Our work has important implications for the design of lubricants, inks, and nanocomposites with tunable viscosity.

cond-mat.soft

Skin formation in evaporating colloidal droplets

When a droplet containing a concentrated suspension evaporates in a dry environment, a layer often forms at the interface accumulating non-volatile material. Such a "skin layer" experiences strong stresses and eventually turns mechanically unstable at the last stage of evaporation. Predicting the formation of such skin layer or particle shell and its properties is a crucial problem for applications and constitutes a multi-scale problem, from the micro/nanoscopic scale of the particles to the millimetric size of the droplets. Interestingly, its physical description lies at the interface between deterministic macroscopic evaporation models and microscopic stochastic particles interactions and diffusion. In this work we present a general theoretical approach to obtain the time-dependent particle concentration profile in an implicit manner, for the general case of diffusion-limited evaporation of spherical droplets, and more generally to all 1D non linear diffusion-limited cases with particles pressure and mobility terms of rational form. This approach is compared successfully to numerical solutions obtained using a finite element solver in the limit of high Péclet numbers, and to 2D Brownian dynamics simulations. Our results show that the concentration profiles and shell formation onset depend nontrivially on the initial packing fraction. By analyzing these profiles, we determine the position where the glassy layer forms, whose formation is expected to play a critical role in shell buckling. This model provides a robust framework for predicting the size and maximum aspect ratio of the resulting clusters.

physics.flu-dyn

Effect of thermal fluctuations on the average shape of a graphene nanosheet suspended in a shear flow

Graphene nanosheets display large hydrodynamic slip lengths in most solvents, and because of this, adopt a stable orientation in a shear flow instead of rotating when thermal fluctuations are negligible [Kamal et al., Nature Comm., 11.1,2020]. In this paper, we combine molecular dynamics simulations and boundary integral simulations to demonstrate that the time-averaged 'S' shape adopted by a flexible graphene nanosheet subject to moderate thermal fluctuation is comparable to the shape predicted when neglecting thermal fluctuations. The stable 'S' shape adopted by the particle results primarily from the normal hydrodynamic traction, which is sensitive to the orientation of the particle with respect to the flow direction. Our results imply that thermally-induced shape fluctuations have a relatively minor effect on the time-averaged rheology of dilute suspensions of graphene nanosheets for relatively large but finite Péclet numbers.

physics.comp-ph

Hindered settling of log-normally distributed particulate suspensions: theoretical models vs. Stokesian simulations

Settling velocity statistics for dilute, non-Brownian suspensions of polydisperse spheres having a log-normal size distribution are analysed by Stokesian Dynamics, as a function of the total volume fraction and width of the size distribution. Several hundred instantaneous configurations are averaged to obtain reliable statistics. Average velocities for each particle class are compared to the models proposed by Batchelor, Richardson & Zaki, Davis & Gecol, and Masliyah-Lockett-Bassoon (MLB). Batchelor's model is shown to give reasonably accurate predictions when the volume fraction is within 5%. Because of its complexity, this model is however hardly used in practice, so lower-order models are needed. We found that while the other hindered settling models can give reasonably accurate predictions of the velocity of the largest particles, all of them overestimate - in certain cases by a large margin - the velocity of the smaller particles. By computing the fluid-particle velocity slip for each particle class and using Batchelor's model, we explain why predicting the lower tail of the particle size distribution is challenging, and propose possible avenues for model improvement. The analysis of velocity fluctuations suggest quantitative similarities between velocity fluctuations in monodisperse and polydisperse suspensions.

physics.flu-dyn

Buckling of a monolayer of plate-like particles trapped at a fluid-fluid interface

Particles trapped at a fluid-fluid interface by capillary forces can form a monolayer that jams and buckles when subject to uni-axial compression. Here we investigate experimentally the buckling mechanics of monolayers of millimeter-sized rigid plates trapped at a planar fluid-fluid interface subject to uni-axial compression in a Langmuir trough. We quantified the buckling wavelength and the associated force on the trough barriers as a function of the degree of compression. To explain the observed buckling wavelength and forces in the two-dimensional monolayer, we consider a simplified system composed of a linear chain of plate-like particles. The chain system enables us to build a theoretical model which is then compared to the two-dimensional monolayer data. Both the experiments and analytical model show that the wavelength of buckling of a monolayer of plate-like particles is of the order of the particle size, a different scaling from the one reported for monolayers of spheres. A simple model of buckling surface pressure is also proposed, and an analysis of the effect of the bending rigidity resulting from a small overlap between nanosheet particles is presented. These results can be applied to the modeling of the interfacial rheology and buckling dynamics of interfacial layers of 2D nanomaterials.

cond-mat.soft

Analysis and optimization of a multicascade method for the size fractionation of poly-dispersed particle systems via sedimentation or centrifugation

Sedimentation and centrifugation can be used to sort particles by size, using a multistep (multicascade) method in which particles in the sediment are removed and the content of the supernatant is processed again, repeating the cycle several times. This paper proposes a theoretical analysis of this process, based on a one-dimensional model, with a view to identify parameters that are optimal to obtain a relatively monodispersed suspension, starting from a log-normal particle size distribution. We found that a rational choice of the sedimentation/centrifugation time enables to control the amount of particles outside of the desired size range (impurities). Surprisingly, the multistep method does not converge, as multiple steps are worse than 2 steps. Band sedimentation, in which a particle-rich layer is overlaid on clear fluid, offers substantial benefits in terms of impurity reduction with respect to starting from a completely mixed situation. An application to graphene fractionation is discussed.

physics.flu-dyn

Hydrodynamic interactions change the buckling threshold of parallel flexible sheets in shear flow

Buckling induced by viscous flow changes the shape of sheet-like nanomaterial particles suspended in liquids. This instability at the particle scale affects collective behavior of suspension flows and has many technological and biological implications. Here, we investigated the effect of viscous hydrodynamic interactions on the morphology of flexible sheets. By analyzing a model experiment using thin sheets suspended in a shear cell, we found that a pair of sheets can bend for a shear rate ten times lower than the buckling threshold defined for a single sheet. This effect is caused by a lateral hydrodynamic force that arises from the disturbance flow field induced by the neighboring sheet. The lateral hydrodynamic force removes the buckling instability but massively enhances the bending deformation. For small separations between sheets, lubrication forces prevail and prevent deformation. Those two opposing effects result in a non-monotonic relation between distances and shear rate for bending. Our study suggests that the morphology of sheet-like particles in suspensions is not purely a material property, but also depends on particle concentration and microstructure.

physics.flu-dyn

Towards nanomechanical models of liquid-phase exfoliation of layered 2D nanomaterials: analysis of a $π$-peel model

In liquid-phase exfoliation for the production of 2D nanomaterials fluid forces are used to gently overcome adhesive interlayer forces, leading to single- or few-layer 2D nanomaterials. Predicting accurately the critical fluid shear rate for exfoliation is a crucial challenge. By combining notions of fluid mechanics and fracture mechanics, we analyse a mathematical model of exfoliation, focusing on the $π$-peel regime in which bending forces are much smaller than the applied hydrodynamic forces. We find that in this regime the shear rate is approximately proportional to the adhesion energy, independent of the bending rigidity of the exfoliated sheet, and inversely proportional to the size $a$ of a (assumed pre-existing) material flaw. The model appears to give values comparable to those obtained in wet ball milling, but to overestimate the shear rate values reported for turbulent exfoliation (by rotor mixing or microfluidization). We suggest that for turbulent exfoliation a "cleavage model" may be more appropriate, as it gives a stronger dependence on $a$ and smaller critical shear rates.

cond-mat.soft

Liquid exfoliation of multilayer graphene in sheared solvents: a molecular dynamics investigation

Liquid-phase exfoliation, the use of a sheared liquid to delaminate graphite into few-layer graphene, is a promising technique for the large-scale production of graphene. But the micro and nanoscale fluid-structure processes controlling the exfoliation are not fully understood. Here we perform non-equilibrium molecular dynamics simulations of a defect-free graphite nanoplatelet suspended in a shear flow and measure the critical shear rate $\dot γ_c$ needed for the exfoliation to occur. We compare $\dot γ_c$ for different solvents including water and NMP, and nanoplatelets of different lengths. Using a theoretical model based on a balance between the work done by viscous shearing forces and the change in interfacial energies upon layer sliding, we are able to predict the critical shear rates $\dot γ_c$ measured in simulations. We find that an accurate prediction of the exfoliation of short graphite nanoplatelets is possible only if both hydrodynamic slip and the fluid forces on the graphene edges are considered, and if an accurate value of the solid-liquid surface energy is used. The commonly used "geometric-mean" approximation for the solid-liquid energy leads to grossly incorrect predictions.

cond-mat.soft

Dynamical Theory of the Inverted Cheerios Effect

Recent experiments have shown that liquid drops on highly deformable substrates exhibit mutual interactions. This is similar to the Cheerios effect, the capillary interaction of solid particles at a liquid interface, but now the roles of solid and liquid are reversed. Here we present a dynamical theory for this inverted Cheerios effect, taking into account elasticity, capillarity and the viscoelastic rheology of the substrate. We compute the velocity at which droplets attract, or repel, as a function of their separation. The theory is compared to a simplified model in which the viscoelastic dissipation is treated as a localized force at the contact line. It is found that the two models differ only at small separation between the droplets, and both of them accurately describe experimental observations.

cond-mat.soft

Dipolar Capillary Interactions between Tilted Ellipsoidal Particles Adsorbed at Fluid-Fluid Interfaces

Capillary interactions have emerged as a tool for the directed assembly of particles adsorbed at fluid-fluid interfaces, and play a role in controlling the mechanical properties of emulsions and foams. In this paper, following Davies et al. [Advanced Materials, 26, 6715 (2014)] investigation into the assembly of ellipsoidal particles at interfaces interacting via dipolar capillary interactions, we numerically investigate the interaction between tilted ellipsoidal particles adsorbed at a fluid-fluid interface as their aspect ratio, tilt angle, bond angle, and separation vary. High-resolution Surface Evolver simulations of ellipsoidal particle pairs in contact reveal an energy barrier between a metastable tip-tip configuration and a stable side-side configuration. The side-side configuration is the global energy minimum for all parameters we investigated. Lattice Boltzmann simulations of clusters of up to 12 ellipsoidal particles show novel highly symmetric flower-like and ring-like arrangements.

cond-mat.soft

Drops on soft solids: Free energy and double transition of contact angles

The equilibrium shape of liquid drops on elastic substrates is determined by minimising elastic and capillary free energies, focusing on thick incompressible substrates. The problem is governed by three length scales: the size of the drop $R$, the molecular size $a$, and the ratio of surface tension to elastic modulus $γ/E$. We show that the contact angles undergo two transitions upon changing the substrates from rigid to soft. The microscopic wetting angles deviate from Young's law when $γ/Ea \gg 1$, while the apparent macroscopic angle only changes in the very soft limit $γ/ER \gg 1$. The elastic deformations are worked out in the simplifying case where the solid surface energy is assumed constant. The total free energy turns out lower on softer substrates, consistent with recent experiments.

physics.flu-dyn