arXiv subjects

Marcello Sega

Publications and source records attributed to Marcello Sega.

At least 19 recordsLinked to original sources

arXiv2025

Hydrogen Bond Topology Reveals Layering of LDL-like and HDL-like Water at its Liquid/Vapor Interface

The discovery of high-density liquid (HDL) and low-density liquid (LDL) water has been a major success of molecular simulations, yet extending this analysis to interfacial water is challenging due to conventional order parameters assuming local homogeneity. This limitation previously prevented resolving the composition of the surface layer of the liquid/vapour interface. Here, we apply a recently introduced topological order parameter [R. Foffi and F. Sciortino, J. Phys. Chem. B 127, 378-386 (2022)] to analyze the composition of the water/vapor interface across a broad temperature range. Our results reveal that LDL-like water dominates the outermost region at all temperatures, while HDL-like water accumulates beneath it, presenting a clear layering roughly below the temperature of maximum density. This structured stratification, previously inaccessible, highlights the power of the topological order parameter in resolving interfacial molecular heterogeneity and provides new insights into the structural properties of water at interfaces.

cond-mat.soft↗

arXiv2023

A sharp interface approach for wetting dynamics of coated droplets and soft particles

The wetting dynamics of liquid particles, from coated droplets to soft capsules, holds significant technological interest. Motivated by the need to simulate liquid metal droplet with an oxidize surface layer, in this work we introduce a computational scheme that allows to simulate droplet dynamics with general surface properties and model different levels of interface stiffness, describing also cases that are intermediate between pure droplets and capsules. Our approach is based on a combination of the immersed boundary (IB) and the lattice Boltzmann (LB) methods. Here, we validate our approach against the theoretical predictions in the context of shear flow and static wetting properties and we show its effectiveness in accessing the wetting dynamics, exploring the ability of the scheme to address a broad phenomenology.

physics.flu-dyn↗

arXiv2023

Suspensions of viscoelastic capsules: effect of membrane viscosity on transient dynamics

Membrane viscosity is known to play a central role in the transient dynamics of isolated viscoelastic capsules by decreasing their deformation, inducing shape oscillations and reducing the loading time, that is, the time required to reach the steady-state deformation. However, for dense suspensions of capsules, our understanding of the influence of the membrane viscosity is minimal. In this work, we perform a systematic numerical investigation based on coupled immersed boundary -- lattice Boltzmann (IB-LB) simulations of viscoelastic spherical capsule suspensions in the non-inertial regime. We show the effect of the membrane viscosity on the transient dynamics as a function of volume fraction and capillary number. Our results indicate that the influence of membrane viscosity on both deformation and loading time strongly depends on the volume fraction in a non-trivial manner: dense suspensions with large surface viscosity are more resistant to deformation but attain loading times that are characteristic of capsules with no surface viscosity, thus opening the possibility to obtain richer combinations of mechanical features.

cond-mat.soft↗

arXiv2023

Viscous to inertial coalescence of liquid lenses: a lattice Boltzmann investigation

Liquid lens coalescence is an important mechanism involved in many industrial and scientific applications. It has been investigated both theoretically and experimentally, yet it is numerically very challenging to obtain consistent results over the wide ranges of surface tension and viscosity values that are necessary to capture the asymptotic temporal behavior in the viscous and inertial limits. We report results of massively parallel simulations based on the color gradient lattice Boltzmann method, which overcome these limitations, and investigate the scaling laws of both regimes. For the two-dimensional case we find good agreement with the similarity solution of the thin-sheet equation, where in the viscous regime the connecting bridge grows linearly with time and in the inertial regime proportionally to $t^{2/3}$. In three dimensions, the viscous growth of the bridge also exhibits a linear time dependence, while in the inertial regime the growth of both the bridge height and the bridge width is proportional to $t^{1/2}$.

physics.flu-dyn↗

arXiv2023

Surface viscosity in simple liquids

The response of Newtonian liquids to small perturbations is usually considered to be fully described by homogeneous transport coefficients like shear and dilatational viscosity. However, the presence of strong density gradients at the liquid/vapor boundary of fluids hints at the possible existence of an inhomogeneous viscosity. Here, we show that a surface viscosity emerges from the collective dynamics of interfacial layers in molecular simulations of simple liquids. We estimate the surface viscosity to be 8-16 times smaller than that of the bulk fluid at the thermodynamic point considered. This result can have important implications for reactions at liquid surfaces in atmospheric chemistry and catalysis.

cond-mat.soft↗

arXiv2022

High-density liquid (HDL) adsorption at the supercooled water/vapor interface and its possible relation to the second surface tension inflection point

We investigate the properties of water along the liquid/vapor coexistence line in the supercooled regime down to the no-man's land. Extensive molecular dynamics simulations of the TIP4P/2005 liquid/vapor interface in the range 198 -- 348 K allow us to locate the second surface tension inflection point with high accuracy at 283$\pm$5 K, close to the temperature of maximum density (TMD). This temperature also coincides with the appearance of a density anomaly at the interface known as the apophysis. We relate the emergence of the apophysis to the observation of HDL water adsorption in the proximity of the liquid/vapor interface.

cond-mat.soft↗

arXiv2022

Resolving the microscopic hydrodynamics at the moving contact line

The molecular structure of moving contact lines (MCLs) and the emergence of a corresponding macroscopic dissipation have made the MCL a paradigm of fluid dynamics. Through novel averaging techniques that remove capillary waves smearing we achieve an unprecedented resolution in molecular dynamics (MD) simulations and find that they match with the continuum description obtained by finite element method (FEM) down to molecular scales. This allows us to distinguish dissipation at the liquid-solid interface (Navier-slip) and at the contact line, the latter being negligible for the rather smooth substrate considered.

cond-mat.soft↗

arXiv2022

Inertial focusing of a dilute suspension in pipe flow

The dynamics of rigid particle suspensions in a wall-bounded laminar flow present several non-trivial and intriguing features, including particle ordering, lateral transport, and the appearance of stable, preferential locations like the Segré-Silberberg annulus. The formation of more than one annulus is a particularly puzzling phenomenon that is still not fully explained. Here, we present numerical simulation results of a dilute suspension of particles in (periodic) pipe flow based on the lattice Boltzmann and the discrete element methods (DEM). Our simulations provide access to the full radial position history of the particles while traveling downstream. This allows to accurately quantify the transient and steady states. We observe the formation of the secondary, inner annulus and show that its position invariably shifts toward the Segré-Silberberg one if the channel is sufficiently long, proving that it is, in fact, a transient feature for Reynolds numbers (Re) up to 600. We quantify the variation of the channel focusing length ($L_s/2R$) with Re. Interestingly and unlike the theoretical prediction for a point-like particle, we observe that $L_s/2R$ increases with Re for both the single particle and the suspension.

physics.flu-dyn↗

arXiv2022

Liquid film rupture beyond the thin-film equation: a multi-component lattice Boltzmann study

Under the condition of partial surface wettability, thin liquid films can be destabilized by small perturbations and rupture into droplets. As successfully predicted by the thin film equation (TFE), the rupture dynamics are dictated by the liquid-solid interaction. The theory describes the latter using the disjoining pressure or, equivalently, the contact angle. The introduction of a secondary fluid can lead to a richer phenomenology thanks to the presence of different fluid/surface interaction energies but has so far not been investigated. In this work, we study the rupture of liquid films with different heights immersed in a secondary fluid using a multi-component lattice Boltzmann (LB) approach. We investigate a wide range of surface interaction energies, equilibrium contact angles, and film thicknesses. We found that the rupture time can differ by about one order of magnitude for identical equilibrium contact angles but different surface free energies. Interestingly, the TFE describes the observed breakup dynamics qualitatively well, up to equilibrium contact angles as large as 130$^\circ$. A small film thickness is a much stricter requirement for the validity of the TFE, and agreement with LB results is found only for ratios $ε=h/L$ of the film height $h$ and lateral system size $L$ such as $ε\lesssim\times10^{-3}$.

physics.flu-dyn↗

arXiv2022

On the accuracy and performance of the lattice Boltzmann method with 64-bit, 32-bit and novel 16-bit number formats

Fluid dynamics simulations with the lattice Boltzmann method (LBM) are very memory-intensive. Alongside reduction in memory footprint, significant performance benefits can be achieved by using FP32 (single) precision compared to FP64 (double) precision, especially on GPUs. Here, we evaluate the possibility to use even FP16 and Posit16 (half) precision for storing fluid populations, while still carrying arithmetic operations in FP32. For this, we first show that the commonly occurring number range in the LBM is a lot smaller than the FP16 number range. Based on this observation, we develop novel 16-bit formats - based on a modified IEEE-754 and on a modified Posit standard - that are specifically tailored to the needs of the LBM. We then carry out an in-depth characterization of LBM accuracy for six different test systems with increasing complexity: Poiseuille flow, Taylor-Green vortices, Karman vortex streets, lid-driven cavity, a microcapsule in shear flow (utilizing the immersed-boundary method) and finally the impact of a raindrop (based on a Volume-of-Fluid approach). We find that the difference in accuracy between FP64 and FP32 is negligible in almost all cases, and that for a large number of cases even 16-bit is sufficient. Finally, we provide a detailed performance analysis of all precision levels on a large number of hardware microarchitectures and show that significant speedup is achieved with mixed FP32/16-bit.

physics.comp-ph↗

arXiv2022

Structure and scaling laws of liquid/vapor interfaces close to the critical point

To reach a deeper understanding of fluid interfaces it is necessary to identify a meaningful coarse-graining length that separates intrinsic fluctuations from capillary ones, given the lack of a proper statistical mechanical definition of the latter. Here, with the help of unsupervised learning techniques, we introduce a new length scale based on the local density of the fluid. This length scale follows a scaling law that diverges more mildly than the bulk correlation length upon approaching the critical point. This allows to distinguish regimes of correlated and uncorrelated capillary waves from that of intrinsic fluctuations.

cond-mat.soft↗

arXiv2021

Capillary interactions, aggregate formation and the rheology of particle-laden flows: a lattice Boltzmann study

The agglomeration of particles caused by the formation of capillary bridges has a decisive impact on the transport properties of a variety of at a first sight very different systems such as capillary suspensions, fluidized beds in chemical reactors, or even sand castles. Here, we study the connection between the microstructure of the agglomerates and the rheology of fluidized suspensions using a coupled lattice Boltzmann and discrete element method approach. We address the influence of the shear rate, the secondary fluid surface tension, and the suspending liquid viscosity. The presence of capillary interactions promotes the formation of either filaments or globular clusters, leading to an increased suspension viscosity. Unexpectedly, filaments have the opposite effect on the viscosity as compared to globular clusters, decreasing the suspension viscosity at larger capillary interaction strengths. In addition, we show that the suspending fluid viscosity also has a non-trivial influence on the effective viscosity of the suspension, a fact usually not taken into account by empirical models.

physics.flu-dyn↗

arXiv2021

Capillary-bridge Forces Between Solid Particles: Insights from Lattice Boltzmann Simulations

Liquid capillary-bridge formation between solid particles has a critical influence on the rheological properties of granular materials and, in particular, on the efficiency of fluidized bed reactors. The available analytical and semi-analytical methods have inherent limitations, and often do not cover important aspects, like the presence of non-axisymmetric bridges. Here, we conduct numerical simulations of the capillary bridge formation between equally and unequally-sized solid particles using the lattice Boltzmann method, and provide an assessment of the accuracy of different families of analytical models. We find that some of the models taken into account are shown to perform better than others. However, all of them fail to predict the capillary force for contact angles larger than $π/2$, where a repulsive capillary force attempts to push the solid particle outwards to minimize the surface energy, especially at a small separation distance.

cond-mat.soft↗

arXiv2021

Lattice Boltzmann simulations of drying suspensions of soft particles

The ordering of particles in the drying process of a colloidal suspension is crucial in determining the properties of the resulting film. For example, microscopic inhomogeneities can lead to the formation of cracks and defects that can deteriorate the quality of the film considerably. This type of problem is inherently multiscale and here we study it numerically, using our recently developed method for the simulation of soft polymeric capsules in multicomponent fluids. We focus on the effect of the particle softness on the film microstructure during the drying phase and how it relates to the formation of defects. We quantify the order of the particles by measuring both the Voronoi entropy and the isotropic order parameter. Surprisingly, both observables exhibit a non-monotonic behaviour when the softness of the particles is increased. We further investigate the correlation between the interparticle interaction and the change in the microstructure during the evaporation phase. We observe that the rigid particles form chain-like structures that tend to scatter into small clusters when the particle softness is increased.

cond-mat.soft↗

arXiv2021

Monolayer Structure of Supramolecular Antagonistic Salt Aggregates

The speculated presence of monomolecular lamellae of antagonistic salts in oil-water mixtures has left several open questions besides their hypothetical existence, including their microscopic structure and stabilization mechanism. Here, we simulate the spontaneous formation of supramolecular aggregates of the antagonistic salt sodium tetraphenylborate (NaBPh$_4$) in water and 3-methylpyridine (3-MP) at the atomistic level. We show that, indeed, the lamellae are formed by a monomolecular layer of the anion, enveloped by 3-MP and hydrated sodium counterions. To understand which thermodynamic forces drive the aggregation, we compare the full-atomistic model with a simplified one for the salt and show that the strong hydrophobic effect granted by the large excluded volume of the anion, together with electrostatic repulsion, suffice to explain the stability of the monomolecular lamellae.

cond-mat.soft↗

arXiv2020

Ab-initio Structure and Thermodynamics of the RPBE-D3 Water/Vapor Interface by Neural-Network Molecular Dynamics

Aided by a neural network representation of the density functional theory (DFT) potential energy landscape of water in the RPBE approximation corrected for dispersion, we calculate several structural and thermodynamic properties of its liquid/vapor interface. The neural network speed allows us to bridge the size and time scale gaps required to sample the properties of water along its liquid/vapor coexistence line with unprecedented precision.

cond-mat.soft↗

arXiv2020

Capillary interactions between soft capsules protruding through thin fluid films

When a suspension dries, the suspending fluid evaporates, leaving behind a dry film composed of the suspended particles. During the final stages of drying, the height of the fluid film on the substrate drops below the particle size, inducing local interface deformations that lead to strong capillary interactions among the particles. Although capillary interactions between rigid particles are well studied, much is still to be understood about the behaviour of soft particles and the role of their softness during the final stages of film drying. Here, we use our recently-introduced numerical method that couples a fluid described using the lattice Boltzmann approach to a finite element description of deformable objects to investigate the drying process of a film with suspended soft particles. Our measured menisci deformations and lateral capillary forces, which agree well with previous theoretical and experimental works in case of rigid particles, show the deformations become smaller with increasing particles softness, resulting in weaker lateral interaction forces. At large interparticle distances, the force approaches that of rigid particles. Finally, we investigate the time dependent formation of particle clusters at the late stages of the film drying.

cond-mat.soft↗

arXiv2020

On the weak scaling of the contact distance between two fluctuating interfaces with system size

A pair of flat parallel surfaces, each freely diffusing along the direction of their separation, will eventually come into contact. If the shapes of these surfaces also fluctuate, then contact will occur when their centers of mass remain separated by a nonzero distance $\ell$. Here we examine the statistics of $\ell$ at the time of first contact for surfaces that evolve in time according to the Edwards-Wilkinson equation. We present a general approach to calculate its probability distribution and determine how its most likely value $\ell^*$ depends on the surfaces' lateral size $L$. We are motivated by an interest in the motion of interfaces between two phases at conditions of thermodynamic coexistence, and in particular the annihilation of domain wall pairs under periodic boundary conditions. Computer simulations of this scenario verify the predicted scaling behavior in two and three dimensions. In the latter case, slow growth where $\ell^\ast$ is an algebraic function of $\log L$ implies that slab-shaped domains remain topologically intact until $\ell$ becomes very small, contradicting expectations from equilibrium thermodynamics.

physics.comp-ph↗