arXiv subjects

Francesco Puosi

Publications and source records attributed to Francesco Puosi.

12 recordsLinked to original sources

arXiv2022

Plastic ridge formation in a compressed thin amorphous film

We demonstrate that surface morphogenesis in compressed thin films may result from spatially correlated plastic activity. A soft glassy film strongly adhering to a smooth and rigid substrate and subjected to uniaxial compression, indeed, does not undergo any global elastic pattern-forming instability, but responds plastically via localized burst events that self-organize, leading to the emergence of a series of parallel ridges transverse to the compression axis. This phenomenon has been completely overlooked, but results from common features of the plastic response of glasses, hence should be highly generic for compressed glassy thin films.

cond-mat.soft↗

arXiv2021

Mutual Information in Molecular and Macromolecular Systems

The relaxation properties of viscous liquids close to their glass transition (GT) have been widely characterised by the statistical tool of time correlation functions. However, the strong influence of ubiquitous non-linearities calls for new, alternative tools of analysis. In this respect, information theory-based observables and, more specifically, mutual information (MI) are gaining increasing interest. Here, we report on novel, deeper insight provided by MI-based analysis of molecular dynamics simulations of molecular and macromolecular glass-formers on two distinct aspects of transport and relaxation close to GT, namely dynamical heterogeneity (DH) and secondary Johari--Goldstein (JG) relaxation processes. In a model molecular liquid with significant DH, MI reveals two populations of particles organised in clusters having either filamentous or compact globular structures that exhibit different mobility and relaxation properties. In a model polymer melt, MI provides clearer evidence of JG secondary relaxation and sharper insight into its DH. It is found that both DH and MI between the orientation and the displacement of the bonds reach (local) maxima at the time scales of the primary and JG secondary relaxation. This suggests that, in (macro)molecular systems, the mechanistic explanation of both DH and relaxation must involve rotation/translation coupling.

cond-mat.soft↗

arXiv2021

Open and anisotropic soft regions in a model polymer glass

The vibrational dynamics of a model polymer glass is studied by Molecular Dynamics simulations. The focus is on the "soft" monomers with high participation to the lower-frequency vibrational modes contributing to the thermodynamic anomalies of glasses. To better evidence their role, the threshold to qualify monomers as soft is made severe, allowing for the use of systems with limited size. A marked tendency of soft monomers to form quasi-local clusters involving up to 15 monomers is evidenced. Each chain contributes to a cluster up to about three monomers and a single cluster involves monomer belonging to about 2-3 chains. Clusters with monomers belonging to a single chain are rare. The open and tenuous character of the clusters is revealed by their fractal dimension $d_f < 2$. The inertia tensor of the soft clusters evidences their strong anisotropy in shape and remarkable linear correlation of the two largest eigenvalues. Owing to the limited size of the system, finite-size effects, as well as dependence of the results on the adopted polymer length, cannot be ruled out.

cond-mat.soft↗

arXiv2021

Johari-Goldstein heterogeneous dynamics in a model polymer

The heterogeneous character of the Johari-Goldstein (JG) relaxation is evidenced by molecular-dynamics simulation of a model polymer system. A double-peaked evolution of dynamic heterogeneity (DH), with maxima located at JG and structural relaxation time scales, is observed and mechanistically explained. {The short-time single-particle displacement during JG relaxation weakly correlates with the long-time one observed during structural relaxation}.

cond-mat.soft↗

arXiv2020

Non-local cooperative atomic motions that govern dissipation in amorphous tantala unveiled by dynamical mechanical spectroscopy

The mechanisms governing mechanical dissipation in amorphous tantala are studied at microscopic scale via Molecular Dynamics simulations, namely by mechanical spectroscopy in a wide range of temperature and frequency. We find that dissipation is associated with irreversible atomic rearrangements with a sharp cooperative character, involving tens to hundreds of atoms arranged in spatially extended clusters of polyhedra. Remarkably, at low temperature we observe an excess of plastically rearranging oxygen atoms which correlates with the experimental peak in the macroscopic mechanical losses. A detailed structural analysis reveals preferential connections of the irreversibly rearranging polyhedra, corresponding to edge and face sharing. These results might lead to microscopically informed design rules for reducing mechanical losses in relevant materials for structural, optical, and sensing applications.

cond-mat.mtrl-sci↗

arXiv2019

Fast Vibrational Modes and Slow Heterogeneous Dynamics in Polymers and Viscous Liquids

Many systems, including polymers and molecular liquids, when adequately cooled and/or compressed, solidify into a disordered solid, i.e., a glass. The~transition is not abrupt, featuring progressive decrease of the microscopic mobility and huge slowing down of the relaxation.} A~distinctive aspect of glass-forming materials is the microscopic dynamical heterogeneity (DH), i.e., the presence of regions with almost immobile particles coexisting with others where highly mobile ones are located. Following the first compelling evidence of a strong correlation between vibrational dynamics and ultraslow relaxation, we posed the question if the vibrational dynamics encodes predictive information on DH. Here, we review our results, drawn from molecular-dynamics numerical simulation of polymeric and molecular glass-formers, with a special focus on both the breakdown of the Stokes--Einstein relation between diffusion and viscosity, and the size of the regions with correlated displacements.

cond-mat.soft↗

arXiv2016

Plastic response and correlations in athermally sheared amorphous solids

The onset of irreversible deformation in low-temperature amorphous solids is due to the accumulation of elementary events, consisting of spacially and temporally localized atomic rearrangements involving only a few tens of atoms. Recently, numerical and experimental work addressed the issue of spatio-temporal correlations between these plastic events. Here, we provide further insight into these correlations by investigating, via molecular dynamics (MD) simulations, the plastic response of a two-dimensional amorphous solid to artificially triggered local shear transformations. We show that while the plastic response is virtually absent in as-quenched configurations, it becomes apparent if a shear strain was previously imposed on the system. Plastic response has a four-fold symmetry which is characteristic of the shear stress redistribution following the local transformation. At high shear rate we report evidence for a fluctuation-dissipation relation, connecting plastic response and correlation, which seems to break down if lower shear rates are considered.

cond-mat.soft↗

arXiv2016

Direct calculation of the critical Casimir force in a binary fluid

We show that critical Casimir effects can be accessed through direct simulation of a model binary fluid passing through the demixing transition. We work in the semi grand canonical ensemble, in slab geometry, in which the Casimir force appears as the excess of the generalized pressure, $P_{\bot}-nμ$. The excesses of the perpendicular pressure, $P_{\bot}$, and of $nμ$, are individually of much larger amplitude. A critical pressure anisotropy is observed between forces parallel and perpendicular to the confinement direction, which collapses onto a universal scaling function closely related to that of the critical Casimir force.

cond-mat.stat-mech↗

arXiv2015

Driving rate dependence of avalanche statistics and shapes at the yielding transition

We study stress time series caused by plastic avalanches in athermally sheared disordered materials. Using particle-based simulations and a mesoscopic elasto-plastic model, we analyze size and shear-rate dependence of the stress-drop durations and size distributions together with their average temporal shape. We find critical exponents different from mean-field predictions, and a clear asymmetry for individual avalanches. We probe scaling relations for the rate dependency of the dynamics and we report a crossover towards mean-field results for strong driving.

cond-mat.soft↗

arXiv2015

Probing relevant ingredients in mean-field approaches for the athermal rheology of yield stress materials

Although the notion of mechanical noise is expected to play a key role in the non-linear rheology of athermally sheared amorphous systems, its characterization has so far remained elusive. Here, we show using molecular dynamic simulations that in spite of the presence of strong spatio-temporal correlations in the system, the local stress exhibits normal diffusion under the effect of the mechanical noise in the finite driving regime. The diffusion constant appears to be proportional to the mean plastic activity. Our data suggests that the corresponding proportionality constant is density independent, and can be directly related to the specific form of the rheological flow curve, pointing the way to a generic way of modeling mechanical noise in mean-field equations.

cond-mat.soft↗

arXiv2015

Elastic consequences of a single plastic event: towards a realistic account of structural disorder and shear wave propagation in models of flowing amorphous solids

Shear transformations (i.e., localised rearrangements of particles resulting in the shear deformation of a small region of the sample) are the building blocks of mesoscale models for the flow of disordered solids. In order to compute the time-dependent response of the solid material to such a shear transformation, with a proper account of elastic heterogeneity and shear wave propagation, we propose and implement a very simple Finite-Element (FE) -based method. Molecular Dynamics (MD) simulations of a binary Lennard-Jones glass are used as a benchmark for comparison, and information about the microscopic viscosity and the local elastic constants is directly extracted from the MD system and used as input in FE. We find very good agreement between FE and MD regarding the temporal evolution of the disorder-averaged displacement field induced by a shear transformation, which turns out to coincide with the response of a uniform elastic medium. However, fluctuations are relatively large, and their magnitude is satisfactorily captured by the FE simulations of an elastically heterogeneous system. Besides, accounting for elastic anisotropy on the mesoscale is not crucial in this respect. The proposed method thus paves the way for models of the rheology of amorphous solids which are both computationally efficient and realistic, in that structural disorder and inertial effects are accounted for.

cond-mat.soft↗

arXiv2014

Time dependent elastic response to a local shear transformation in amorphous solids

The elastic response of a two-dimensional amorphous solid to induced local shear transformations, which mimic the elementary plastic events occurring in deformed glasses, is investigated via Molecular Dynamics simulations. We show that for different spatial realizations of the transformation, despite relative fluctuations of order one, the long time equilibrium response averages out to the prediction of the Eshelby inclusion problem for a continuum elastic medium. We characterize the effects of the underlying dynamics on the propagation of the elastic signal. A crossover from a propagative transmission in the case of weakly-damped dynamics to a diffusive transmission for strong damping is evidenced. In the latter case, the full time dependent elastic response is in agreement with the theoretical prediction, obtained by solving the diffusion equation for the displacement field in an elastic medium.

cond-mat.soft↗