Searcharxiv⌕ Search

arXiv subjects

A. Zaccone

Publications and source records attributed to A. Zaccone.

At least 19 recordsLinked to original sources
arXiv2026

Ultrastable 2D glasses and packings explained by local centrosymmetry

Using the most recent numerical data by Bolton-Lum \emph{et al.} [Phys. Rev. Lett. 136, 058201 (2026)], we demonstrate that ideal ultrastable glasses in the athermal limit (or ultrastable ideal 2D disk packings) possess a remarkably high degree of local centrosymmetry. In particular, we find that the inversion-symmetry order parameter for local force transmission introduced in Milkus and Zaccone, [Phys. Rev. 93, 094204 (2016)], is as high as $F_{IS}= 0.84522$, to be compared with $F_{IS}=1$ for perfect centrosymmetric crystals free of defects, and with $F_{IS} \sim 0.3-0.5$ for standard random packings. This observation provides a clear, natural explanation for the ultra-high shear modulus of ideal packings and ideal glasses, because the high centrosymmetry prevents non-affine relaxations which decrease the shear modulus. The same mechanism explains the absence of boson peak-like soft vibrational modes. These results also confirm what was found previous work, i.e. that the bond-orientational order parameter is a very poor correlator for the vibrational and mechanical

cond-mat.soft↗
arXiv2025

Amorphous Solid Model of Vectorial Hopfield Neural Networks

We introduce a three-dimensional vectorial extension of the Hopfield associative-memory model in which each neuron is a unit vector on $S^2$ and synaptic couplings are $3\times 3$ blocks generated through a vectorial Hebbian rule. The resulting block-structured operator is mathematically analogous to the Hessian of amorphous solids and induces a rigid energy landscape with deep minima for stored patterns. Simulations and spectral analysis show that the vectorial network substantially outperforms the classical binary Hopfield model. For moderate connectivity, the critical storage ratio $\gamma_c$ grows approximately linearly with the coordination number $Z$, while for $Z\gtrsim 40$ a high-connectivity regime emerges in which $\gamma_c$ systematically exceeds the extrapolated low-$Z$ linear fit. At the same time, a persistent spectral gap separates pattern modes from the bulk and basins of attraction enlarge, yielding enhanced robustness to initialization noise. Thus geometric constraints combined with amorphous-solid-inspired structure produce associative memories with superior storage and retrieval performance, especially in the high-connectivity ($Z \gtrsim 20$-$30$) regime.

cond-mat.dis-nn↗
arXiv2024

Low-Temperature Heat Transport under Phonon Confinement in Nanostructures

Heat transport in bulk materials is well described using the Debye theory of 3D vibrational modes (phonons) and the acoustic match model. However, in cryogenic nanodevices, phonon wavelengths exceed device dimensions, leading to confinement effects that standard models fail to address. With the growing application of low-temperature devices in communication, sensing, and quantum technologies, there is an urgent need for models that accurately describe heat transport under confinement. We introduce a computational approach to obtain phonon heat capacity and heat transport rates between solids in various confined geometries, that can be easily integrated into, e.g., the standard two-temperature model. Confinement significantly reduces heat capacity and may slow down heat transport. We have validated our model in experiments on strongly disordered NbTiN superconducting nanostructures, widely used in highly efficient single-photon detectors, and we argue that confinement is due to their polycrystalline granular structure. These findings point to potential advances in cryogenic device performance through tailored material and microstructure engineering.

cond-mat.mes-hall↗
arXiv2023

Shear flow of non-Brownian rod-sphere mixtures near jamming

We use the discrete element method, taking particle contact and hydrodynamic lubrication into account, to unveil the shear rheology of suspensions of frictionless non-Brownian rods in the dense packing fraction regime. We find that, analogously to the random close packing volume fraction, the shear-driven jamming point of this system varies in a non-monotonic fashion as a function of the rod aspect ratio. The latter strongly influences how the addition of rod-like particles affects the rheological response of a suspension of frictionless non-Brownian spheres to an external shear flow. At fixed values of the total (rods plus spheres) packing fraction, the viscosity of the suspension is reduced by the addition of "short" ( $\leq 2$) rods but is instead increased by the addition of "long" ( $\geq2$) rods. A mechanistic interpretation is provided in terms of packing and excluded-volume arguments.

cond-mat.soft↗
arXiv2023

Molecular-level relation between intra-particle glass transition temperature and stability of colloidal suspensions

In many colloidal suspensions, the dispersed colloidal particles are amorphous solids resulting from vitrification. A crucial open problem is understanding how colloidal stability is affected by the intra-particle glass transition. By dealing with the latter process from a solid-state perspective, we estabilish a proportionality relation between the intra-particle glass transition temperature, $T_{\textrm{g}},$ and the Hamaker constant, $A_\textrm{H},$ of a generic suspension of nanoparticles. It follows that $T_\textrm{g}$ can be used as a convenient parameter (alternative to $A_\textrm{H}$) for controlling the stability of colloidal systems. Within DLVO theory, we show that the novel relationship, connecting $T_\textrm{g}$ to $A_\textrm{H},$ implies the critical coagulation ionic strength (CCIS) to be a monotonically decreasing function of $T_{\textrm{g}}.$ We connect our predictions to recent experimental findings.

cond-mat.soft↗
arXiv2022

Thermal expansion and the glass transition

Melting is well understood in terms of the Lindemann criterion, essentially stating that crystalline materials melt when the thermal vibrations of their atoms become such vigorous that they shake themselves free of the binding forces. However, how about another common type of solids: glasses, where the nature of the solid-liquid crossover is highly controversial? The Lindemann criterion implies that the thermal expansion coefficients alpha of crystals are inversely proportional to their melting temperatures. Here we find that, unexpectedly, alpha of glasses decreases much stronger with increasing glass-transition temperature Tg marking the liquid-solid crossover in this material class. However, scaling alpha by the fragility m, a measure of particle cooperativity, restores the proportionality, i.e., alpha/m ~ 1/Tg. Obviously, for a glass to become liquid, it is not sufficient to simply overcome the interparticle binding energies. Instead, more energy has to be invested to break up the typical cooperative particle network which is considered a hallmark feature of glassy materials. Surprisingly, alpha of the liquid phase reveals similar anomalous behaviour and is universally enhanced by a constant factor of ~3. The found universalities allow estimating glass-transition temperatures from thermal expansion and vice versa.

cond-mat.dis-nn↗
arXiv2021

Slow stretched-exponential and fast compressed-exponential relaxation from local event dynamics

We propose an atomistic model for correlated particle dynamics in liquids and glasses predicting both slow stretched-exponential relaxation (SER) and fast compressed-exponential relaxation (CER). The model is based on the key concept of elastically interacting local relaxation events. SER is related to slowing down of dynamics of local relaxation events as a result of this interaction, whereas CER is related to the avalanche-like dynamics in the low-temperature glass state. The model predicts temperature dependence of SER and CER seen experimentally and recovers the simple, Debye, exponential decay at high temperature. Finally, we reproduce SER to CER crossover across the glass transition recently observed in metallic glasses.

cond-mat.stat-mech↗
arXiv2021

Universal $L^{-3}$ finite-size effects in the viscoelasticity of confined amorphous systems

We present a theory of viscoelasticity of amorphous media, which takes into account the effects of confinement along one of three spatial dimensions. The framework is based on the nonaffine extension of lattice dynamics to amorphous systems, or nonaffine response theory. The size effects due to the confinement are taken into account via the nonaffine part of the shear storage modulus $G'$. The nonaffine contribution is written as a sum over modes in $k$-space. With a rigorous argument based on the analysis of the $k$-space integral over modes, it is shown that the confinement size $L$ in one spatial dimension, e.g. the $z$ axis, leads to a infrared cut-off for the modes contributing to the nonaffine (softening) correction to the modulus that scales as $L^{-3}$. Corrections for finite sample size $D$ in the two perpendicular dimensions scale as $\sim (L/D)^4$, and are negligible for $L \ll D$. For liquids it is predicted that $G'\sim L^{-3}$ in agreement with a previous more approximate analysis, whereas for amorphous materials $G' \sim G'_{bulk} + βL^{-3}$. For the case of liquids, four different experimental systems are shown to be very well described by the $L^{-3}$ law.

cond-mat.soft↗
arXiv2020

Low-energy optical phonons induce glassy-like vibrational and thermal anomalies in ordered crystals

It is widely accepted that structural glasses and disordered crystals exhibit anomalies in the their thermal, mechanical and acoustic properties as manifestations of the breakdown of the long-wavelength approximation in a disordered dissipative environment. However, the same type of glassy-like anomalies (i.e. boson peak in the vibrational density of states (VDOS) above the Debye level, peak in the normalized specific heat at $T\simeq10 K$ etc) have been recently observed also in perfectly ordered crystals, including thermoelectric compounds. Here we present a theory that predicts these surprising effects in perfectly ordered crystals as a result of low-lying (soft) optical phonons. In particular, it is seen that a strong boson peak anomaly (low-energy excess of modes) in the VDOS can be due almost entirely to the presence of low-energy optical phonons, provided that their energy is comparable to that of the acoustic modes at the Brillouin zone boundary. The boson peak is predicted also to occur in the heat capacity at low $T$. In presence of strong damping (which might be due to anharmonicities in the ordered crystals), these optical phonons contribute to the low-$T$ deviation from Debye's $T^{3}$ law, producing a linear-in-$T$ behavior which is typical of glasses, even though no assumptions of disorder whatsoever are made in the model. These findings are relevant for understanding and tuning thermal transport properties of thermoelectric compounds, and possibly for the enhancement of electron-phonon superconductivity.

cond-mat.mtrl-sci↗
arXiv2019

Radial distribution function of Lennard-Jones fluids in shear flows from intermediate asymptotics

Determining the microstructure of colloidal suspensions under shear flows has been a challenge for theoretical and computational methods due to the singularly-perturbed boundary-layer nature of the problem. Previous approaches have been limited to the case of hard-sphere systems and suffer from various limitations in their applicability. We present a new analytic scheme based on intermediate asymptotics which solves the Smoluchowski diffusion-convection equation including both intermolecular and hydrodynamic interactions. The method is able to recover previous results for the hard-sphere fluid and, for the first time, to predict the radial distribution function (rdf) of attractive fluids such as the Lennard-Jones (LJ) fluid. In particular, a new depletion effect is predicted in the rdf of the LJ fluid under shear. This method can be used for the theoretical modelling and understanding of real fluids subjected to flow, with applications ranging from chemical systems to colloids, rheology, plasmas, and atmospherical science.

cond-mat.soft↗
arXiv2018

Disentangling $α$ and $β$ relaxation in orientationally disordered crystals with theory and experiments

We use a microscopically motivated Generalized Langevin Equation (GLE) approach to link the vibrational density of states (VDOS) to the dielectric response of orientational glasses (OGs). The dielectric function calculated based on the GLE is compared with experimental data for the paradigmatic case of two OGs: Freon 112 and Freon 113, around and just above $T_g$. The memory function is related to the integral of the VDOS times a spectral coupling function $γ(ω_p)$, which tells the degree of dynamical coupling between molecular degrees of freedom at different eigenfrequencies. The comparative analysis of the two Freons reveals that the appearance of a secondary $β$ relaxation in Freon 112 is due to cooperative dynamical coupling in the regime of mesoscopic motions caused by stronger anharmonicity (absent in Freon 113), and is associated with comparatively lower boson peak in the VDOS. The proposed framework brings together all the key aspects of glassy physics (VDOS with boson peak, dynamical heterogeneity, dissipation, anharmonicity) into a single model.

cond-mat.soft↗
arXiv2017

Disentangling interatomic repulsion and anharmonicity in the viscosity and fragility of glasses

Within the shoving model of the glass transition, the relaxation time and the viscosity are related to the local cage rigidity. This approach can be extended down to the atomic-level in terms of the interatomic interaction, or potential of mean-force. We applied this approach to both real metallic glass-formers and model Lennard-Jones glasses. The main outcome of this analysis is that in metallic glasses the thermal expansion contribution is mostly independent of composition and is uncorrelated with the interatomic repulsion: as a consequence, the fragility increases upon increasing the interatomic repulsion steepness. In the Lennard-Jones glasses, the scenario is opposite: thermal expansion and interatomic repulsion contributions are strongly correlated, and the fragility decreases upon increasing the repulsion steepness. This framework allows one to tell apart systems where "soft atoms make strong glasses" from those where, instead, "soft atoms make fragile glasses". Hence, it opens up the way for the rational, atomistic tuning of the fragility and viscosity of widely different glass-forming materials all the way from strong to fragile.

cond-mat.soft↗
arXiv2017

Direct link between boson-peak modes and dielectric $α$-relaxation in glasses

We compute the dielectric response of glasses starting from a microscopic system-bath Hamiltonian of the Zwanzig-Caldeira-Leggett type and using an ansatz from kinetic theory for the memory function in the resulting Generalized Langevin Equation. The resulting framework requires the knowledge of the vibrational density of states (DOS) as input, that we take from numerical evaluation of a marginally-stable harmonic disordered lattice, featuring a strong boson peak (excess of soft modes over Debye $\simω_{p}^{2}$ law). The dielectric function calculated based on this ansatz is compared with experimental data for the paradigmatic case of glycerol at $T\lesssim T_{g}$. Good agreement is found for both the reactive (real part) of the response and for the $α$-relaxation peak in the imaginary part, with a significant improvement over earlier theoretical approaches, especially in the reactive modulus. On the low-frequency side of the $α$-peak, the fitting supports the presence of $\sim ω_{p}^{4}$ modes at vanishing eigenfrequency as recently shown in [Phys. Rev. Lett. 117, 035501 (2016)]. $α$-wing asymmetry and stretched-exponential behaviour are recovered by our framework, which shows that these features are, to a large extent, caused by the soft boson-peak modes in the DOS.

cond-mat.soft↗
arXiv2017

The relation between stretched-exponential relaxation and the vibrational density of states in glassy disordered systems

Amorphous solids or glasses are known to exhibit stretched-exponential decay over broad time intervals in several of their macroscopic observables: intermediate scattering function, dielectric relaxation modulus, time-elastic modulus etc. This behaviour is prominent especially near the glass transition. In this Letter we show, on the example of dielectric relaxation, that stretched-exponential relaxation is intimately related to the peculiar lattice dynamics of glasses. By reformulating the Lorentz model of dielectric matter in a more general form, we express the dielectric response as a function of the vibrational density of states (DOS) for a random assembly of spherical particles interacting harmonically with their nearest-neighbours. Surprisingly we find that near the glass transition for this system (which coincides with the Maxwell rigidity transition), the dielectric relaxation is perfectly consistent with stretched-exponential behaviour with Kohlrausch exponents $0.56 < β< 0.65$, which is the range where exponents are measured in most experimental systems. Crucially, the root cause of stretched-exponential relaxation can be traced back to soft modes (boson-peak) in the DOS.

cond-mat.soft↗
arXiv2016

Kinetics of fragmentation and dissociation of two-strand protein filaments: Coarse-grained simulations and experiments

While a significant body of investigations have been focused on the process of protein self-assembly, much less is understood about the reverse process of a filament breaking due to thermal motion into smaller fragments, or depolymerization of subunits from the filament ends. Indirect evidence for actin and amyloid filament fragmentation has been reported, although the phenomenon has never been directly observed either experimentally or in simulations. Here we report the direct observation of filament depolymerization and breakup in a minimal, calibrated model of coarse-grained molecular simulation. We quantify the orders of magnitude by which the depolymerization rate from the filament ends $k_\mathrm{off}$ is larger than fragmentation rate $k_{-}$ and establish the law $k_\mathrm{off}/k_- = \exp [( \varepsilon_\| - \varepsilon_\bot) / k_\mathrm{B}T ] = \exp [0.5 \varepsilon / k_\mathrm{B}T ]$, which accounts for the topology and energy of bonds holding the filament together. This mechanism and the order-of-magnitude predictions are well supported by direct experimental measurements of depolymerization of insulin amyloid filaments.

cond-mat.soft↗
arXiv2016

Population-balance description of shear-induced clustering, gelation and suspension viscosity in sheared DLVO colloids

Application of shear flow to charge-stabilized aqueous colloidal suspensions is ubiquitous in industrial applications and as a means to achieve controlled field-induced assembly of nanoparticles. Yet, applying shear flow to a charge-stabilized colloidal suspension, which is initially monodisperse and in quasi-equilibrium leads to non-trivial clustering phenomena (and sometimes to a gelation transition), dominated by the complex interplay between DLVO interactions and shear flow. The quantitative understanding of these strongly nonequilibrium phenomena is still far from being complete. By taking advantage of a recent shear-induced aggregation rate theory developed in our group, we present here a systematic numerical study, based on the governing master kinetic equation (population-balance) for the shear-induced clustering and breakup of colloids exposed to shear flow. In the presence of sufficiently stable particles, the clustering kinetics is characterized by an initial very slow growth, controlled by repulsion. During this regime, particles are slowly aggregating to form clusters, the reactivity of which increases along with their size growth. When their size reaches a critical threshold, a very rapid, explosive-like growth follows, where shear forces are able to overcome the energy barrier between particles. This stage terminates when a dynamic balance between shear-induced aggregation and cluster breakage is reached. It is also observed that these systems are characterized by a cluster mass distribution that for a long time presents a well-defined bimodality. The model predictions are quantitatively in excellent agreement with available experimental data, showing how the theoretical picture is able to quantitatively account for the underlying nonequilibrum physics.

cond-mat.soft↗
arXiv2016

Effects of shear flow on phase nucleation and crystallization

Classical nucleation theory offers a good framework for understanding the common features of new phase formation processes in metastable homogeneous media at rest. However, nucleation processes in liquids are ubiquitously affected by hydrodynamic flow, and there is no satisfactory understanding of whether shear promotes or slows down the nucleation process. We developed a classical nucleation theory for sheared systems starting from the molecular level of the Becker-Doering master kinetic equation and we analytically derived a closed-form expression for the nucleation rate. The theory accounts for the effect of flow-mediated transport of molecules to the nucleus of the new phase, as well as for the mechanical deformation imparted to the nucleus by the flow field. The competition between flow-induced molecular transport, which accelerates nucleation, and flow-induced nucleus straining, which lowers the nucleation rate by increasing the nucleation energy barrier, gives rise to a marked nonmonotonic dependence of the nucleation rate on the shear rate. The theory predicts an optimal shear rate at which the nucleation rate is one order of magnitude larger than in the absence of flow.

cond-mat.soft↗