arXiv subjects

Emanuela Del Gado

Publications and source records attributed to Emanuela Del Gado.

At least 37 records · Page 2Linked to original sources

arXiv2021

The physics of cement cohesion

Cement is one of the most produced materials in the world. A major player in greenhouse gas emissions, it is the main binding agent in concrete, to which it provides a cohesive strength that rapidly increases during setting. Understanding how such cohesion emerges has been a major obstacle to advances in cement science and technology. Here, we combine computational statistical mechanics and theory to demonstrate how cement cohesion results from the organization of interlocked ions and water, progressively confined in nano-slits between charged surfaces of Calcium-Silicate-Hydrates. Due to the water/ions interlocking, dielectric screening is drastically reduced and ionic correlations are proven significantly stronger than previously thought, dictating the evolution of the nano-scale interactions during cement hydration. By developing a quantitative analytical prediction of cement cohesion based on Coulombic forces, we reconcile a novel fundamental understanding of cement hydration with the fully atomistic description of the solid cement paste and open new paths for science and technologies of construction materials.

physics.app-ph↗

arXiv2021

Microscopic interactions and emerging elasticity in model soft particulate gels

We discuss a class of models for particulate gels in which the particle contacts are described by an effective interaction combining a two-body attraction and a three-body angular repulsion. Using molecular dynamics, we show how varying the model parameters allows us to sample, for a given gelation protocol, a variety of gel morphologies. For a specific set of the model parameters, we identify the local elastic structures that get interlocked in the gel network. Using the analytical expression of their elastic energy from the microscopic interactions, we can estimate their contribution to the emergent elasticity of the gel and gain new insight into its origin.

cond-mat.soft↗

arXiv2019

Multi-component colloidal gels: interplay between structure and mechanical proprieties

We present a detailed numerical study of multi-component colloidal gels interacting sterically and obtained by arrested phase separation. Under deformation, we found that the interplay between the different intertwined networks is key. Increasing the number of component leads to softer solids that can accomodate progressively larger strain before yielding. The simulations highlight how this is the direct consequence of the purely repulsive interactions between the different components, which end up enhancing the linear response of the material. Our work {provides new insight into mechanisms at play for controlling the material properties and open the road to new design principles for} soft composite solids

cond-mat.soft↗

arXiv2019

A computational study of transient shear banding in soft jammed solids

We have designed 3D numerical simulations of a soft spheres model, with size polidispersity and in athermal conditions, to study the transient shear banding that occurs during yielding of jammed soft solids. We analyze the effects of different types of drag coefficients used in the simulations and compare the results obtained using Lees-Edwards periodic boundary conditions with the case in which the same model solid is confined between two walls. The specific damping mechanism and the different boundary conditions indeed modify the load curves and the velocity profiles in the transient regime. Nevertheless, we find that the presence of a stress-overshoot and of a related transient banding phenomenon for large enough samples are a robust feature for overdamped systems, where their presence do not depend on the specific drag used and on the different boundary conditions.

cond-mat.soft↗

arXiv2018

Correlated rigidity percolation and colloidal gels

Rigidity percolation (RP) occurs when mechanical stability emerges in disordered networks as constraints or components are added. Here we discuss RP with structural correlations, an effect ignored in classical theories albeit relevant to many liquid-to-amorphous-solid transitions, such as colloidal gelation, which are due to attractive interactions and aggregation. Using a lattice model, we show that structural correlations shift RP to lower volume fractions. Through molecular dynamics simulations, we show that increasing attraction in colloidal gelation increases structural correlation and thus lowers the RP transition, agreeing with experiments. Hence colloidal gelation can be understood as a RP transition, but occurs at volume fractions far below values predicted by the classical RP, due to attractive interactions which induce structural correlation.

cond-mat.soft↗

arXiv2018

Computing the linear viscoelastic properties of soft gels using an Optimally Windowed Chirp protocol

We use molecular dynamics simulations of a model three-dimensional particulate gel, to investigate the linear viscoelastic response. The numerical simulations are combined with a novel test protocol (the optimally- windowed chirp or OWCh), in which a continuous exponentially-varying frequency sweep windowed by a tapered cosine function is applied. The mechanical response of the gel is then analyzed in the Fourier domain. We show that i) OWCh leads to an accurate computation of the full frequency spectrum at a rate significantly faster than with the traditional discrete frequency sweeps, and with a reasonably high signal-to-noise ratio, and ii) the bulk viscoelastic response of the microscopic model can be described in terms of a simple mesoscopic constitutive model. The simulated gel response is in fact well described by a mechanical model corresponding to a fractional Kelvin-Voigt model with a single Scott-Blair (or springpot) element and a spring in parallel. By varying the viscous damping and the particle mass used in the microscopic simulations over a wide range of values, we demonstrate the existence of a single master curve for the frequency dependence of the viscoelastic response of the gel that is fully predicted by the constitutive model. By developing a fast and robust protocol for evaluating the linear viscoelastic spectrum of these soft solids, we open the path towards novel multiscale insight into the rheological response for such complex materials.

cond-mat.soft↗

arXiv2017

Network topology in soft gels: hardening and softening materials

The structural complexity of soft gels is at the origin of a versatile mechanical response that allows for large deformations, controlled elastic recovery and toughness in the same material. A limit to exploiting the potential of such materials is the insufficient fundamental understanding of the microstructural origin of the bulk mechanical properties. Here we investigate the role of the network topology in a model gel through 3D numerical simulations. Our study links the topology of the network organization in space to its non-linear rheological response preceding yielding and damage: our analysis elucidates how the network connectivity alone could be used to modify the gel mechanics at large strains, from strain-softening to hardening and even to a brittle response. These findings provide new insight for smart material design and for understanding the non-trivial mechanical response of a potentially wide range of technologically relevant materials.

cond-mat.soft↗

arXiv2017

Emergence and persistence of flow inhomogeneities in the yielding and fluidization of dense soft solids

The response to shear of the dense soft solids features a stress overshoot and a persistent shear banding before reaching a homogeneously flowing state. In 3D large scale simulations we analyze the time required for the onset of homogeneous flow, the normal stresses and structural signatures at different shear rates and in different flow geometries, finding that the stress overshoot, the shear band formation and its persistence are controlled by the presence of overconstrained microscopic domains in the initially solid samples. Being able to identify such domains in our model by prevalently icosahedrally packed regions, we show that they allow for stress accumulation during the stress overshoot and that their structural reorganization controls the emergence and the persistence of the shear banding.

cond-mat.soft↗

arXiv2017

Elastically driven, intermittent microscopic dynamics in soft solids

Soft solids with tunable mechanical response are at the core of new material technologies, but a crucial limit for applications is their progressive aging over time, which dramatically affects their functionalities. The generally accepted paradigm is that such aging is gradual and its origin is in slower than exponential microscopic dynamics, akin to the ones in supercooled liquids or glasses. Nevertheless, time- and space-resolved measurements have provided contrasting evidence: dynamics faster than exponential, intermittency, and abrupt structural changes. Here we use 3D computer simulations of a microscopic model to reveal that the timescales governing stress relaxation respectively through thermal fluctuations and elastic recovery are key for the aging dynamics. When thermal fluctuations are too weak, stress heterogeneities frozen-in upon solidification can still partially relax through elastically driven fluctuations. Such fluctuations are intermittent, because of strong correlations that persist over the timescale of experiments or simulations, leading to faster than exponential dynamics.

cond-mat.soft↗

arXiv2016

Making soft solids flow: microscopic bursts and conga lines in jammed emulsions

It is well known that jammed soft materials will flow if sheared above their yield stress - think mayonnaise spread on bread - but a complete microscopic description of this seemingly sim- ple process has yet to emerge. What remains elusive is a microscopic framework that explains the macroscopic flow, derived from a 3-D spatially resolved analysis of the dynamics of the droplets or particles that compose the soft material. By combining confocal-rheology experiments on compressed emulsions and numerical simulations, we unravel that the primary microscopic mechanisms for flow are strongly influenced by the rate of the imposed deformation. When shearing fast, small coordinated clusters of droplets move collectively as in a conga line, while at low rates the flow emerges from bursts of droplet rearrangements, correlated over large domains. These regions exhibit complex spatio-temporal correlation patterns that reflect the long range elasticity embedded in the jammed material. These results identify the three-dimensional structure of microscopic rearrangements within sheared soft solids, revealing that the characteristic shape and dynamics of these structures are strongly determined by the rate of the external shear.

cond-mat.soft↗

arXiv2014

Self-assembly and cooperative dynamics of a model colloidal gel network

We study the assembly into a gel network of colloidal particles, via effective interactions that yield local rigidity and make dilute network structures mechanically stable. The self-assembly process can be described by a Flory-Huggins theory, until a network of chains forms, whose mesh size is on the order of, or smaller than, the persistence length of the chains. The localization of the particles in the network, akin to some extent to caging in dense glasses, is determined by the network topology, and the network restructuring, which takes place via bond breaking and recombination, is characterized by highly cooperative dynamics. We use NVE and NVT Molecular Dynamics as well as Langevin Dynamics and find a qualitatively similar time dependence of time correlations and of the dynamical susceptibility of the restructuring gel. This confirms that the cooperative dynamics emerge from the mesoscale organization of the network.

cond-mat.soft↗

arXiv2014

Microscopic Picture of Cooperative Processes in Restructuring Gel Networks

Colloidal gel networks are disordered elastic solids that can form even in extremely dilute particle suspensions. With interaction strengths comparable to the thermal energy, their stress-bearing network can locally restructure via breaking and reforming interparticle bonds. This allows for yielding, self-healing, and adaptive mechanics under deformation. Designing such features requires controlling stress transmission through the complex structure of the gel and this is challenging because the link between local restructuring and overall response of the network is still missing. Here, we use a space resolved analysis of dynamical processes and numerical simulations of a model gel to gain insight into this link. We show that consequences of local bond breaking propagate along the gel network over distances larger than the average mesh size. This provides the missing microscopic explanation for why nonlocal constitutive relations are necessary to rationalize the nontrivial mechanical response of colloidal gels.

cond-mat.soft↗

arXiv2014

Stress localization, stiffening and yielding in a model colloidal gel

We use numerical simulations and an athermal quasi-static shear protocol to investigate the yielding of a model colloidal gel. Under increasing deformation, the elastic regime is followed by a significant stiffening before yielding takes place. A space-resolved analysis of deformations and stresses unravel how the complex load curve observed is the result of stress localization and that the yielding can take place by breaking a very small fraction of the network connections. The stiffening corresponds to the stretching of the network chains, unbent and aligned along the direction of maximum extension. It is characterized by a strong localization of tensile stresses, that triggers the breaking of a few network nodes at around 30% of strain. Increasing deformation favors further breaking but also shear-induced bonding, eventually leading to a large-scale reorganization of the gel structure at the yielding. At low enough shear rates, density and velocity profiles display significant spatial inhomogeneity during yielding in agreement with experimental observations.

cond-mat.soft↗

arXiv2014

Soft modes and non-affine rearrangements in the inherent structures of supercooled liquids

We find that the hierarchical organization of the potential energy landscape in a model supercooled liquid can be related to a change in the spatial distribution of soft normal modes. For groups of nearby minima, between which fast relaxation processes typically occur, the localization of the soft modes is very similar. The spatial distribution of soft regions changes, instead, for minima between which transitions relevant to structural relaxation occur. This may be the reason why the soft modes are able to predict spatial heterogeneities in the dynamics. Nevertheless, the very softest modes are only weakly correlated with dynamical heterogeneities, and instead show higher statistical overlap with regions in the local minima that would undergo non-affine rearrangements if subjected to a shear deformation. This feature of the supercooled liquid is reminiscent of the behavior of non-affine deformations in amorphous solids, where the very softest modes identify the {\it loci} of plastic instabilities.

cond-mat.dis-nn↗

arXiv2013

Unexpected decoupling of stretching and bending modes in protein gels

We show that gels formed by arrested spinodal decomposition of protein solutions exhibit elastic properties in two distinct frequency domains, both elastic moduli exhibiting a remarkably strong dependence on volume fraction. Considering the large difference between the protein size and the characteristic length of the network we model the gels as porous media and show that the high and low frequency elastic moduli can be respectively attributed to stretching and bending modes. The unexpected decoupling of the two modes in the frequency domain is attributed to the length scale involved: while stretching mainly relates to the relative displacement of two particles, bending involves the deformation of a strand with a thickness of the order of a thousand particle diameters.

cond-mat.soft↗

arXiv2012

Deformation of inherent structures to detect long-range correlations in supercooled liquids

We propose deformations of inherent structures as a suitable tool for detecting structural changes underlying the onset of cooperativity in supercooled liquids. The non-affine displacement (NAD) field resulting from the applied deformation shows characteristic differences between the high temperature liquid and supercooled state, that are typically observed in dynamic quantities. The average magnitude of the NAD is very sensitive to temperature changes in the supercooled regime and is found to be strongly correlated with the inherent structure energy. In addition, the NAD field is characterized by a correlation length that increases upon lowering the temperature towards the supercooled regime.

cond-mat.dis-nn↗

arXiv2011

Shear-driven solidification of dilute colloidal suspensions

We show that the shear-induced solidification of dilute charge-stabilized (DLVO) colloids is due to the interplay between the shear-induced formation and breakage of large non-Brownian clusters. While their size is limited by breakage, their number density increases with the shearing-time. Upon flow cessation, the dense packing of clusters interconnects into a rigid state by means of grainy bonds, each involving a large number of primary colloidal bonds. The emerging picture of shear-driven solidification in dilute colloidal suspensions combines the gelation of Brownian systems with the jamming of athermal systems.

cond-mat.soft↗

arXiv2010

Scaling between Structural Relaxation and Particle Caging in a Model Colloidal Gel

In polymers melts and supercooled liquids, the glassy dynamics is characterized by the rattling of monomers or particles in the cage formed by their neighbors. Recently, a direct correlation in such systems, described by a universal scaling form, has been established between the rattling amplitude and the structural relaxation time. In this paper we analyze the glassy dynamics emerging from the formation of a persistent network in a model colloidal gel at very low density. The structural relaxation time of the gel network is compared with the mean squared displacement at short times, corresponding to the localization length associated to the presence of energetic bonds. Interestingly, we find that the same type of scaling as for the dense glassy systems holds. Our findings well elucidate the strong coupling between the cooperative rearrangements of the gel network and the single particle localization in the structure. Our results further indicate that the scaling captures indeed fundamental physical elements of glassy dynamics.

cond-mat.soft↗