arXiv subjects

Emanuela Del Gado

Publications and source records attributed to Emanuela Del Gado.

At least 19 recordsLinked to original sources

arXiv2026

Investigating the Nature of Discontinuous Shear Thickening: Beyond a Mean-Field Description

Dense suspensions can undergo a dramatic increase in viscosity at a critical value of the shear stress. This phenomenon, termed discontinuous shear thickening (DST), has been attributed to an increase in the fraction of particle interactions becoming frictional with increasing shear stress, and a successful mean-field theory has been developed to explain various accompanying rheological properties. On a microscopic scale, however, conventional structural analysis measures such as the grain-position pair correlation function show no significant changes with the onset of DST, though recent work has shown that similar analysis in the dual space of contact forces does lead to marked changes at this transition. Furthermore, experimental results have suggested the existence of higher-order microscopic correlations and the importance of incorporating fluctuations away from a mean-field description. To this end, we use a higher-order cluster analysis tool to study the force networks obtained from simulations of dense suspensions to construct an effective interaction potential in force space. We show that there are significant changes occurring in this potential as a function of density and stress close to DST. We discuss the implications of these observations on an emergent field theory of the DST transition.

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arXiv2026

Geomimicry: Emergent Dynamics in Earth-Mediated Complex Materials

Soils and sediments are soft, amorphous materials with complex microstructures and mechanical properties, that are also building blocks for industrial materials such as concrete. These Earth-mediated materials evolve under prolonged environmental pressures like mechanical stress, chemical gradients, and biological activity. Here, we introduce geomimicry, a new paradigm for designing sustainable materials by learning from the emergent and adaptive dynamics of Earth-mediated matter. Drawing a parallel to biomimicry, we posit that these geomaterials follow evolutionary design rules, adapting their structure and function in response to persistent natural forces through locally evolved interactions and compositions. Our central argument is that by decoding these rules - primarily through understanding the emergence of novel exotic properties from multiscale interactions between heterogenous components - we can engineer a new class of adaptive, sustainable matter. We propose two complementary approaches here. The top-down approach looks to nature to identify building blocks and map them to functional groups defined by their mechanical behaviors, and then examine how environmental training tunes interactions among these groups. The bottom up approach seeks to leverage and test this framework, building earth materials one component at a time under fluctuating environmental stresses that guide assembly of complex and out-of-equilibrium materials. The goal is to create materials with programmed functionalities, such as erosion resistance or self-healing capabilities. Geomimicry offers a pathway to re-imagine climate-resilient soils and precision agriculture to new insights into planetary terraforming, fundamentally shifting the focus from static compositions to dynamic, evolving systems that are mediated via their environment.

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arXiv2026

Disentangling microstructural elements of shear thickening suspensions via computer simulations of a minimal model

We use a minimal model for a dense suspension undergoing thickening and thinning to investigate microstructural changes in 2d simulations. Our simulations show that in steady flow the contact network contains distinct building blocks which are clearly signaled by sharp peaks in the radial distribution function, similar to what is observed in granular jamming. These structures {deform} during thinning. Non-Gaussian stress fluctuations that only emerge during thickening are associated to power law tails in the distribution of local contact forces, which tend to emerge when the flow-induced building blocks form large spanning assemblies. The subset of the contact network characterized by strong contact forces and connectivity large enough to be rigid or over-constrained is increasingly likely to percolate as the system starts to thicken, and to percolate over larger strain windows during thickening. The tendency of these structures to span the sample and to persist is dramatically reduced during thinning, where instead their deformation allows for a more homogeneous spatial redistribution of contact forces, significantly reducing the fluctuations of the macroscopic stress over time.

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arXiv2025

Exploring the Nonlinear Rheology of Composite Hydrogels: A New Paradigm for LAOS Analysis

We investigate composite biopolymer networks composed of co-polymerized fibrin and gelatin networks and perform rheological measurements over a broad parameter space including strain amplitudes that go beyond the linear response regime. One goal of the work presented here is to provide a prototypical biocomposite material with highly separable polymerization times and controlled nonlinear rheological characteristics. We then extend the Sequence of Physical Processes (SPP)\cite{Rogers2017} into a statistical and geometrical framework that fingerprints the nonlinear rheological response of biopolymer composite gels. Our analysis is based on the changes in the shape of the time-dependent Cole-Cole plots that allow to reduce the time resolved analysis of the SPP method into the transition between linear and nonlinear behavior as the rheological parameters are varied. While the results clearly highlight how the mechanical responses of individual constituents are not simply additive, our extended SPP analysis provides a robust and intuitive classification scheme for comparing the nonlinear response of composite materials subjected to large oscillatory strain.

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arXiv2025

Pinch-point Singularities in Stress-Stress Correlations Reveal Rigidity in Colloidal Gels

We demonstrate that the spatial correlations of microscopic stresses in 2D model colloidal gels obtained in computer simulations can be quantitatively described by the predictions of a theory for emergent elasticity of pre-stressed solids (vector charge theory). By combining a rigidity analysis with the characterization provided by the stress correlations, we show that the theoretical predictions are able to distinguish rigid from floppy gels, and quantify that distinction in terms of the size of a pinch-point singularity emerging at large length scales, which, in the theory, directly derives from the constraints imposed by mechanical equilibrium on the internal forces. We also use the theoretical predictions to investigate the coupling between stress-transmission and rigidity, and we explore the possibility of a Debye-like screening mechanism that would modify the theory predictions below a characteristic length scale.

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arXiv2024

Inter-Species Interactions in Dual, Fibrous Gel Enable Control of Gel Structure and Rheology

Natural and synthetic multi-component gels display emergent properties, which implies that they are more than just the sum of their components. This warrants the investigation of the role played by inter-species interactions in shaping gel architecture and rheology. Here, using computer simulations, we investigate the effect of changing the strength of the interaction between two species forming a fibrous double network. Simply changing the strength of inter-species lateral association, we generate two types of gels: one in which the two components demix, and another one in which the two species wrap around each other. We show that demixed gels have structure and rheology that are largely unaffected by the strength of attraction between the components. In contrast, architecture and material properties of intertwined gels strongly depend on inter-species "stickiness" and volume exclusion. These results can be used as the basis of a design principle for double networks which are made to emphasize either stability to perturbations or responsiveness to stimuli. Similar ideas could be used to interpret naturally occurring multi-component gels.

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arXiv2024

Topological Data Analysis for Particulate Gels

Soft gels, formed via the self-assembly of particulate organic materials, exhibit intricate multi-scale structures that provides them with flexibility and resilience when subjected to external stresses. This work combines molecular simulations and topological data analysis (TDA) to characterize the complex multi-scale structure of soft gels. Our TDA analysis focuses on the use of the Euler characteristic, which is an interpretable and computationally-scalable topological descriptor that is combined with filtration operations to obtain information on the geometric (local) and topological (global) structure of soft gels. We reduce the topological information obtained with TDA using principal component analysis (PCA) and show that this provides an informative low-dimensional representation of gel structure. We use the proposed computational framework to investigate the influence of gel preparation (e.g., quench rate, volume fraction) on soft gel structure and to explore dynamic deformations that emerge under oscillatory shear in various response regimes (linear, nonlinear, and flow). Our analysis identifies specific scales and extents at which hierarchical structures in soft gels are affected; moreover, correlations between structural deformations and mechanical phenomena (such as shear stiffening) are explored. In summary, we show that TDA facilitates the mathematical representation, quantification, and analysis of soft gel structures, extending traditional network analysis methods to capture both local and global organization.

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arXiv2023

Ductile-to-brittle transition and yielding in soft amorphous materials: perspectives and open questions

Soft amorphous materials are viscoelastic solids ubiquitously found around us, from clays and cementitious pastes to emulsions and physical gels encountered in food or biomedical engineering. Under an external deformation, these materials undergo a noteworthy transition from a solid to a liquid state that reshapes the material microstructure. This yielding transition was the main theme of a workshop held from January 9 to 13, 2023 at the Lorentz Center in Leiden. The manuscript presented here offers a critical perspective on the subject, synthesizing insights from the various brainstorming sessions and informal discussions that unfolded during this week of vibrant exchange of ideas. The result of these exchanges takes the form of a series of open questions that represent outstanding experimental, numerical, and theoretical challenges to be tackled in the near future.

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arXiv2023

Memory of shear flow in soft jammed materials

Cessation of flow in simple yield stress fluids results in a complex stress relaxation process that depends on the preceding flow conditions and leads to finite residual stresses. To assess the microscopic origin of this phenomenon, we combine experiments with largescale computer simulations, exploring the behavior of jammed suspensions of soft repulsive particles. A spatio-temporal analysis of microscopic particle motion and local particle configurations reveals two contributions to stress relaxation. One is due to flow induced accumulation of elastic stresses in domains of a given size, which effectively sets the unbalanced stress configurations that trigger correlated dynamics upon flow cessation. This scenario is supported by the observation that the range of spatial correlations of quasi-ballistic displacements obtained upon flow cessation almost exactly mirrors those obtained during flow. The second contribution results from the particle packing that reorganize to minimize the resistance to flow by decreasing the number of locally stiffer configurations. Regaining rigidity upon flow cessation then effectively sets the magnitude of the residual stress. Our findings highlight that flow in yield stress fluids can be seen as a training process during which the material stores information of the flowing state through the development of domains of correlated particle displacements and the reorganization of particle packings optimized to sustain the flow. This encoded memory can then be retrieved in flow cessation experiments.

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arXiv2023

Soft matter physics of the ground beneath our feet

Inspired by presentations by the authors during a workshop organized at the Princeton Center for Theoretical Science (PCTS) in January 2022, we present a perspective on some of the outstanding questions related to the "physics of the ground beneath our feet." These identified challenges are intrinsically shared with the field of Soft Matter but also have unique aspects when the natural environment is studied.

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arXiv2023

Universal scaling of shear thickening transitions

Nearly all dense suspensions undergo dramatic and abrupt thickening transitions in their flow behaviour when sheared at high stresses. Such transitions occur when the dominant interactions between the suspended particles shift from hydrodynamic to frictional. Here, we interpret abrupt shear thickening as a precursor to a rigidity transition and give a complete theory of the viscosity in terms of a universal crossover scaling function from the frictionless jamming point to a rigidity transition associated with friction, anisotropy, and shear. Strikingly, we find experimentally that for two different systems -- cornstarch in glycerol and silica spheres in glycerol -- the viscosity can be collapsed onto a single universal curve over a wide range of stresses and volume fractions. The collapse reveals two separate scaling regimes, due to a crossover between frictionless isotropic jamming and frictional shear jamming, with different critical exponents. The material-specific behaviour due to the microscale particle interactions is incorporated into a scaling variable governing the proximity to shear jamming that depends on both stress and volume fraction. This reformulation opens the door to importing the vast theoretical machinery developed to understand equilibrium critical phenomena to elucidate fundamental physical aspects of the shear thickening transition.

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arXiv2022

The hidden hierarchical nature of soft particulate gels

Soft particulate gels include materials we can eat, squeeze, or 3D print. From foods to bio-inks to cement hydrates, these gels are composed of a small amount of particulate matter (proteins, polymers, colloidal particles, or agglomerates of various origins) embedded in a continuous fluid phase. The solid components assemble to form a porous matrix, providing rigidity and control of the mechanical response, despite being the minority constituent. The rheological response and gel elasticity are direct functions of the particle volume fraction $ϕ$: however, the diverse range of different functional dependencies reported experimentally has, to date, challenged efforts to identify general scaling laws. Here we reveal a hidden hierarchical organization of fractal elements that controls the viscoelastic spectrum, and which is associated with the spatial heterogeneity of the solid matrix topology. The fractal elements form the foundations of a viscoelastic master curve, which we construct using large-scale 3D microscopic simulations of model gels, and can be described by a recursive rheological ladder model over a range of particle volume fractions and gelation rates. The hierarchy of the fractal elements provides the missing general framework required to predict the gel elasticity and the viscoelastic response of these ubiquitous complex materials.

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arXiv2022

Time-resolved microstructural changes in large amplitude oscillatory shear of model single and double component soft gels

Soft particulate gels can reversibly yield when sufficient deformation is applied, and the characteristics of this transition can be enhanced or limited by designing hybrid hydrogel composites. While the microscopic dynamics and macroscopic rheology of these systems have been studied separately in detail, the development of direct connections between the two has been difficult, particularly with regard to the non-linear rheology. To bridge this gap, we perform a series of large amplitude oscillatory shear (LAOS) numerical measurements on model soft particulate gels at different volume fractions using coarse-grained molecular dynamics simulations. We first study a particulate network with local bending stiffness and then we combine it with a second component that can provide additional crosslinking to obtain two-component networks. Through the sequence of physical processes (SPP) framework we define time-resolved dynamic moduli and, by tracking the changes in these moduli through the period, we can distinguish transitions in the material behavior as a function of time. This approach helps us establish the microsopic origin of the non-linear rheology by connecting the changes in dynamic moduli to the corresponding microstructural changes during the deformation including the non-affine displacement of particles, and the breakage, formation, and orientation of bonds.

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arXiv2022

Stress-stress Correlations Reveal Force Chains in Gels

We investigate the spatial correlations of microscopic stresses in soft particulate gels, using 2D and 3D numerical simulations. We use a recently developed theoretical framework predicting the analytical form of stress-stress correlations in amorphous assemblies of athermal grains that acquire rigidity under an external load. These correlations exhibit a pinch-point singularity in Fourier space leading to long-range correlations and strong anisotropy in real space, which are at the origin of force-chains in granular solids. Our analysis for the model particulate gels at low particle volume fractions demonstrates that stress-stress correlations in these soft materials have characteristics very similar to those in granular solids and can be used to identify force chains. We show that the stress-stress correlations can distinguish floppy from rigid gel networks and the intensity patterns reflect changes in shear moduli and network topology, due to the emergence of rigid structures during solidification.

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arXiv2022

Flow induced rigidity percolation in shear thickening suspensions

Discontinuous shear thickening (DST) is associated with a sharp rise of a suspension's viscosity with increasing applied shear rate. A key signature of DST, highlighted in recent studies, is the very large fluctuations of the measured stress as the suspension thickens. A clear link between microstructural development and the dramatic increase of the stress fluctuations has not been established yet. To identify the microstructural underpinnings of this behavior, we perform simulations of sheared dense suspensions. By analyzing particle contact networks, we identify a subset of constrained particles that contribute directly to the rapid rise in viscosity and the large stress fluctuations. Indeed, both phenomena can be explained by the growth and percolation of constrained particle networks -- in direct analogy to rigidity percolation. A finite size scaling analysis confirms this is a percolation phenomenon and allows us to estimate the critical exponents. Our findings reveal the specific microstructural transition that underlies DST.

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arXiv2022

Ion specificity of confined ion-water structuring and nanoscale surface forces in clays

Ion specificity and related Hofmeister effects, ubiquitous in aqueous systems, can have spectacular consequences in hydrated clays, where ion-specific nanoscale surface forces can determine large scale cohesive, swelling and shrinkage behaviors of soil and sediments. We have used a semi-atomistic computational approach and examined sodium, calcium and aluminum counterions confined with water between charged surfaces representative of clay materials, to show that ion-water structuring in nanoscale confinement is at the origin of surface forces between clay particles which are intrinsically ion-specific. When charged surfaces strongly confine ions and water, the amplitude and oscillations of the net pressure naturally emerge from the interplay of electrostatics and steric effects, which can not be captured by existing theories. Increasing confinement and surface charge densities promote ion-water structures that increasingly deviate from the ions' bulk hydration shells, being strongly anisotropic and persistent, and self-organizing into optimized, nearly solid-like assemblies where hardly any free water is left. In these conditions, strongly attractive interactions can prevail between charged surfaces, due to the dramatically reduced dielectric screening of water and the highly organized water-ion structures. By unravelling the ion-specific nature of these nanoscale interactions, we provide evidence that ion-specific solvation structures determined by confinement are at the origin of ion specificity in clays and potentially a broader range of confined aqueous systems.

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arXiv2022

Ordered domains in sheared dense suspensions: the link to viscosity and the disruptive effect of friction

Monodisperse suspensions of Brownian colloidal spheres crystallize at high densities, and ordering under shear has been observed at densities below the crystallization threshold. We perform large-scale simulations of a model suspension containing over $10^5$ particles to quantitatively study the ordering under shear and to investigate its link to the rheological properties of the suspension. We find that at high rates, for $Pe>1$, the shear flow induces an ordering transition that significantly decreases the measured viscosity. This ordering is analyzed in terms of the development of layering and planar order, and we determine that particles are packed into hexagonal crystal layers (with numerous defects) that slide past each other. By computing local $ψ_6$ and $ψ_4$ order parameters, we determine that the defects correspond to chains of particles in a square-like lattice. We compute the individual particle contributions to the stress tensor and discover that the largest contributors to the shear stress are primarily located in these lower density, defect regions. The defect structure enables the formation of compressed chains of particles to resist the shear, but these chains are transient and short-lived. The inclusion of a contact friction force allows the stress-bearing structures to grow into a system-spanning network, thereby disrupting the order and drastically increasing the suspension viscosity.

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arXiv2021

Prestressed elasticity of amorphous solids

Prestress in amorphous solids bears the memory of their formation, and plays a profound role in their mechanical properties, from stiffening or softening elastic moduli to shifting frequencies of vibrational modes, as well as directing yielding and solidification in the nonlinear regime. Here we develop a set of mathematical tools to investigate elasticity of prestressed discrete networks, which disentangles the effects from disorder in configuration and disorder in prestress. Applying these methods to prestressed triangular lattices and a computational model of amorphous solids, we demonstrate the importance of prestress on elasticity, and reveal a number of intriguing effects caused by prestress, including strong spatial heterogeneity in stress-response unique to prestressed solids, power-law distribution of minimal dipole stiffness, and a new criterion to classify floppy modes.

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