arXiv subjects

Samy Merabia

Publications and source records attributed to Samy Merabia.

At least 37 records · Page 2Linked to original sources

arXiv2022

Chapter: Energy conversion at water-solid interfaces using electrokinetic effects

Our Society is in high need of alternatives to fossil fuels. Nanoporous systems filled with aqueous electrolytes show great promises for harvesting the osmotic energy of sea water or waste heat. At the core of energy conversion in such nanofluidic systems lie the so-called electrokinetic effects, coupling thermodynamic gradients and fluxes of different types (hydrodynamical, electrical, chemical, thermal) at electrified water-solid interfaces. This chapter starts by introducing the framework of linear irreversible thermodynamics, and how the latter can be used to describe the direct and coupled responses of a fluidic system, providing general relations between the different response coefficients. The chapter then focuses on the so-called osmotic flows, generated by non-hydrodynamic actuation at liquid-solid interfaces, and illustrate how the induced fluxes can be related to the microscopic properties of the water-solid interface. Finally, the chapter moves to electricity production from non-electric actuation, and discusses in particular the performance of nanofluidic systems for the harvesting of osmotic energy and waste heat.

physics.flu-dyn↗

arXiv2022

Interplay of electron and phonon channels in the refrigeration through molecular junctions

Due to their structured density of states, molecular junctions provide rich resources to filter and control the flow of electrons and phonons. Here we compute the out of equilibrium current-voltage characteristics and dissipated heat of some recently synthesized oligophenylenes (OPE3) using the Density Functional based Tight-Binding (DFTB) method within Non-Equilibrium Green's Function Theory (NEGF). We analyze the Peltier cooling power for these molecular junctions as function of a bias voltage and investigate the parameters that lead to optimal cooling performance. In order to quantify the attainable temperature reduction, an electro-thermal circuit model is presented, in which the key electronic and thermal transport parameters enter. Overall, our results demonstrate that the studied OPE3 devices are compatible with temperature reductions of several K. Based on the results, some strategies to enable high performance devices for cooling applications are briefly discussed.

cond-mat.mes-hall↗

arXiv2021

Fast and Versatile Thermo-osmotic Flows with a Pinch of Salt

Thermo-osmotic flows - flows generated in micro and nanofluidic systems by thermal gradients - could provide an alternative approach to harvest waste heat. However, such use would require massive thermo-osmotic flows, which are up to now only predicted for special and expensive materials. There is thus an urgent need to design affordable nanofluidic systems displaying large thermo-osmotic coefficients. In this paper we propose a general model for thermo-osmosis of aqueous electrolytes in charged nanofluidic channels, taking into account hydrodynamic slip, together with the different solvent and solute contributions to the thermo-osmotic response. We apply this model to a wide range of systems, by studying the effect of wetting, salt type and concentration, and surface charge. We show that intense thermo-osmotic flows can be generated using slipping charged surfaces. We also predict for intermediate wettings a transition from a thermophobic to a thermophilic behavior depending on the surface charge and salt concentration. Overall, this theoretical framework opens an avenue for controlling and manipulating thermally induced flows with common charged surfaces and a pinch of salt.

physics.flu-dyn↗

arXiv2021

Enhanced local viscosity around colloidal nanoparticles probed by Equilibrium Molecular Dynamics Simulations

Nanofluids; dispersions of nanometer-sized particles in a liquid medium; have been proposed for a wide variety of thermal management applications. It is known that a solid-like nanolayer of liquid of typical thickness 0.5-1 nm surrounding the colloidal nanoparticles can act as a thermal bridge between the nanoparticle and the bulk liquid. Yet, its effect on the nanofluid viscosity has not been elucidated so far. In this article, we compute the local viscosity of the nanolayer using equilibrium molecular dynamics based on the Green-Kubo formula. We first assess the validity of the method to predict the viscosity locally. We apply this methodology to the calculation of the local viscosity in the immediate vicinity of a metallic nanoparticle for a wide range of solid-liquid interaction strength, where a nanolayer of thickness 1 nm is observed as a result of the interaction with the nanoparticle. The viscosity of the nanolayer, which is found to be higher than its corresponding bulk value, is directly dependent on the solid-liquid interaction strength. We discuss the origin of this viscosity enhancement and show that the liquid density increment alone cannot explain the values of the viscosity observed. Rather, we suggest that the solid-like structure of the distribution of the liquid atoms in the vicinity of the nanoparticle contributes to the nanolayer viscosity enhancement. Finally, we observe a failure of the Stokes-Einstein relation between viscosity and diffusion close to the wall, depending on the liquid-solid interaction strength, which we rationalize in terms of hydrodynamic slip.

cond-mat.soft↗

arXiv2021

Theoretical framework for the atomistic modeling of frequency-dependent liquid-solid friction

Nanofluidics shows great promise for energy conversion and desalination applications. The performance of nanofluidic devices is controlled by liquid-solid friction, quantified by the Navier friction coefficient (FC). Despite decades of research, there is no well-established generic framework to determine the frequency dependent Navier FC from atomistic simulations. Here, we have derived analytical expressions to connect the Navier FC to the random force autocorrelation on the confining wall, from the observation that the random force autocorrelation can be related to the hydrodynamic boundary condition, where the Navier FC appears. The analytical framework is generic in the sense that it explicitly includes the system size dependence and also the frequency dependence of the FC, which enabled us to address (i) the long-standing plateau issue in the evaluation of the FC and (ii) the non-Markovian behavior of liquid-solid friction of a Lennard-Jones liquid and of water on various walls and at various temperatures, including the supercooled regime. This new framework opens the way to explore the frequency dependent FC for a wide range of complex liquids.

cond-mat.soft↗

arXiv2021

Strong and fast rising pressure waves emitted by plasmonic vapor nanobubbles

Plasmonic vapour nanobubbles are currently considered for a wide variety of applications ranging from solar energy harvesting and photoacoustic imaging to nanoparticle-assisted cancer therapy. Yet, due their small size and unstable nature, their generation and consequences remain difficult to characterize. Here, building on a phase-field model, we report on the existence of strong pressure waves that are emitted when vapor nanobubbles first form around a laser-heated nanoparticle immersed in water, and subsequently after bubble rebound. These effects are strongest when the fluid is locally brought high in its supercritical state, which may be realized with a short laser pulse. Because of the highly out-of-equilibrium nature of nanobubble generation, the waves combine a high pressure peak with a fast pressure rising time, and propagate in water over micron distances, opening the way to induce spatially and temporally localized damage. Discussing the consequences on biological cell membranes, we conclude that acoustic-mediated perforation is more efficient than nanobubble expansion to breach membrane. Our findings should serve as guide for optimizing the thermoacoustic conversion efficiency of plasmonic vapor nanobubbles.

physics.optics↗

arXiv2020

Fast Increase of Nanofluidic Slip in Supercooled Water: the Key Role of Dynamics

Nanofluidics is an emerging field offering innovative solutions for energy harvesting and desalination. The efficiency of these applications depends strongly on liquid-solid slip, arising from a favorable ratio between viscosity and interfacial friction. Using molecular dynamics simulations, we show that wall slip increases strongly when water is cooled below its melting point. For water on graphene, the slip length is multiplied by up to a factor of five and reaches $230$nm at the lowest simulated temperature, $T \sim 225$K; experiments in nanopores can reach much lower temperatures and could reveal even more drastic changes. The predicted fast increase in water slip can also be detected at supercoolings reached experimentally in bulk water, as well as in droplets flowing on anti-icing surfaces. We explain the anomalous slip behavior in the supercooled regime by a decoupling between viscosity and bulk density relaxation dynamics, and we rationalize the wall-type dependency of the enhancement in terms of interfacial density relaxation dynamics. By providing fundamental insights on the molecular mechanisms of hydrodynamic transport in both interfacial and bulk water in the supercooled regime, this study is relevant to the design of anti-icing surfaces and it also paves the way to explore new behaviors in supercooled nanofluidic systems.

cond-mat.soft↗

arXiv2019

Enhanced heat transfer with core-shell metal dielectric nanoparticles

Heat transfer from irradiated metallic nanoparticles is relevant to a broad array of applications ranging from water desalination to photoacoustics. The efficacy of such processes relies on the ability of these nanoparticles to absorb the pulsed illuminating light and to quickly transfer energy to the environment. Here we show that compared to homogeneous gold nanoparticles having the same size, gold-silica core-shell nanoparticles enable heat transfers to liquid water that are faster. We reach this conclusion by considering both analytical and numerical calculations. The key factor explaining enhanced heat transfer is the direct interfacial coupling between metal electrons and silica phonons. We discuss how to obtain fast heating of water in the vicinity of the particle and show that optimal conditions involve nanoparticles with thin silica shells irradiated by ultrafast laser pulses. Our findings should serve as guides for the optimization of thermoplasmonic applications of core-shell nanoparticles.

cond-mat.mtrl-sci↗

arXiv2019

Giant thermoelectric response of nanofluidic systems driven by water excess enthalpy

Nanofluidic systems could in principle be used to produce electricity from waste heat, but current theoretical descriptions predict a rather poor performance as compared to thermoelectric solid materials. Here we investigate the thermoelectric response of NaCl and NaI solutions confined between charged walls, using molecular dynamics simulations. We compute a giant thermoelectric response, two orders of magnitude larger than the predictions of standard models. We show that water excess enthalpy -- neglected in the standard picture -- plays a dominant role in combination with the electroosmotic mobility of the liquid-solid interface. Accordingly, the thermoelectric response can be boosted using surfaces with large hydrodynamic slip. Overall, the heat harvesting performance of the model systems considered here is comparable to that of the best thermoelectric materials, and the fundamental insight provided by molecular dynamics suggests guidelines to further optimize the performance, opening the way to recycle waste heat using nanofluidic devices.

cond-mat.stat-mech↗

arXiv2019

Thermal transport at a nanoparticle-water interface: A molecular dynamics and continuum modeling study

Heat transfer between a silver nanoparticle and surrounding water has been studied using molecular dynamics (MD) simulations. The thermal conductance (Kapitza conductance) at the interface between a nanoparticle and surrounding water has been calculated using four different approaches: transient with/without temperature gradient (internal thermal resistance) in the nanoparticle, steady-state non-equilibrium and finally equilibrium simulations. The results of steady-state non-equilibrium and equilibrium are in agreement but differ from the transient approach results. MD simulations results also reveal that in the quenching process of a hot silver nanoparticle, heat dissipates into the solvent over a length-scale of ~ 2nm and over a timescale of less than 5ps. By introducing a continuum solid-like model and considering a heat conduction mechanism in water, it is observed that the results of the temperature distribution for water shells around the nanoparticle agree well with MD results. It is also found that the local water thermal conductivity around the nanoparticle is greater by about 50 percent than that of bulk water. These results have important implications for understanding heat transfer mechanisms in nanofluids systems and also for cancer photothermal therapy, wherein an accurate local description of heat transfer in an aqueous environment is crucial.

cond-mat.mtrl-sci↗

arXiv2017

Critical angle for interfacial phonon scattering: Results from ab initio lattice dynamics calculations

Thermal boundary resistance is a critical quantity that controls heat transfer at the nanoscale, which is primarily related to interfacial phonon scattering. Here, we combine lattice dynamics calculations and inputs from first principles ab initio simulations to predict phonon transmission at the Si/Ge interface as a function of both the phonon frequency and the phonon wavevector. This technique allows us to determine the overall thermal transmission coefficient as a function of the phonon scattering direction and frequency. Our results show that the thermal energy transmission is highly anisotropic, while thermal energy reflection is almost isotropic. In addition, we found the existence of a global critical angle of transmission beyond which almost no thermal energy is transmitted. This critical angle around 50 degrees is found to be almost independent of the interaction range between Si and Ge, the interfacial bonding strength, and the temperature above 30 K. We interpret these results by carrying out a spectral and angular analysis of the phonon transmission coefficient and differential thermal boundary conductance.

cond-mat.mes-hall↗

arXiv2017

What controls thermo-osmosis? Molecular simulations show the critical role of interfacial hydrodynamics

Thermo-osmotic and related thermo-phoretic phenomena can be found in many situations from biology to colloid science, but the underlying molecular mechanisms remain largely unexplored. Using molecular dynamics simulations, we measured the thermo-osmosis coefficient by both mechano-caloric and thermo-osmotic routes, for different solid-liquid interfacial energies. The simulations reveal in particular the crucial role of nanoscale interfacial hydrodynamics. For non-wetting surfaces , thermo-osmotic transport is largely amplified by hydrodynamic slip at the interface. For wetting surfaces, the position of the hydrodynamic shear plane plays a key role in determining the amplitude and sign of the thermo-osmosis coefficient. Finally, we measure a giant thermo-osmotic response of the water-graphene interface, which we relate to the very low interfacial friction displayed by this system. These results open new perspectives for the design of efficient functional interfaces for, e.g., waste heat harvesting.

cond-mat.soft↗

arXiv2017

Gibbs adsorption impact on a nanodroplet shape: modification of Young-Laplace equation

An efficient technique for the evaluation of the Gibbs adsorption of a liquid on a solid substrate is presented. The behavior of a water nanodroplet on a silicon surface is simulated with molecular dynamics. An external field with varying strength is applied on the system to tune the solid-liquid interfacial contact area. A linear dependence of droplet's volume on the contact area is observed. Our modified Young--Laplace equation is used to explain the influence of the Gibbs adsorption on the nanodroplet volume contraction. Fitting of the molecular dynamics results with these of an analytical approach allows us to evaluate the number of atoms per unit area adsorbed on the substrate, which quantifies the Gibbs adsorption. Thus, a threshold of a droplet size is obtained, for which the impact of the adsorption is crucial. Moreover, the presented results can be applied for the evaluation of the adsorption impact on the physical--chemical properties of systems with important surface-to-volume fraction.

cond-mat.soft↗

arXiv2017

Assessment of elastic models in supercooled water: A molecular dynamics study with the TIP4P/2005f force field

Glass formers exhibit a viscoelastic behavior: at the laboratory timescale, they behave like (glassy) solids at low temperatures, and like liquids at high temperatures. Based on this observation, elastic models relate the long time supercooled dynamics to short time elastic properties of the supercooled liquid. In the present work, we assess the validity of elastic models for the shear viscosity and the $α$-relaxation time of supercooled water, using molecular dynamics simulations with the TIP4P/2005f force field over a wide range of temperatures. We show that elastic models provide a good description of supercooled water dynamics. For the viscosity, two different regimes are observed and the crossover temperature is found to be close to the one where the Stokes-Einstein relation starts to be violated. Our simulations show that only shear properties are important to characterize the effective flow activation energy. This study calls for experimental determination of the high frequency elastic properties of water at low temperatures.

physics.chem-ph↗

arXiv2016

Creep and fluidization in thermal amorphous solids

When submitted to a constant mechanical load, many amorphous solids display power law creep followed by fluidization. A fundamental understanding of these processes is still far from being achieved. Here, we characterize creep and fluidization on the basis of a mesoscopic viscoplastic model that includes thermally activated yielding events and a broad distribution of energy barriers, which may be lowered under the effect of a local deformation. We relate the creep exponent observed before fluidization to the width of barrier distribution and to the specific form of stress redistribution following yielding events. We show that Andrade creep is accompanied by local strain-hardening driven by stress redistribution and find that the fluidization depends exponentially on the applied stress. The simulation results are interpreted in the light of a mean-field analysis, and should help in rationalizing the creep phenomenology of amorphous solids.

cond-mat.soft↗

arXiv2015

Thermal boundary conductance across rough interfaces probed by molecular dynamics

In this article, we report the influence of the interfacial roughness on the thermal boundary conductance between two crystals, using molecular dynamics. We show evidence of a transition between two regimes, depending on the interfacial roughness: when the roughness is small, the boundary conductance is constant taking values close to the conductance of the corresponding planar interface. When the roughness is larger, the conductance becomes larger than the planar interface conductance, and the relative increase is found to be close to the increase of the interfacial area. The cross-plane conductivity of a superlattice with rough interfaces is found to increase in a comparable amount, suggesting that heat transport in superlattices is mainly controlled by the boundary conductance. These observations are interpreted using the wave characteristics of the energy carriers. We characterize also the effect of the angle of the asperities, and find that the boundary conductance displayed by interfaces having steep slopes may become important if the lateral period characterizing the interfacial profile is large enough. Finally, we consider the effect of the shape of the interfaces, and show that the sinusoidal interface displays the highest conductance, because of its large true interfacial area. All these considerations are relevant to the optimization of nanoscale interfacial energy transport.

cond-mat.mtrl-sci↗

arXiv2013

Numerical study of a slip-link model for polymer melts and nanocomposites

We present a numerical study of the slip link model introduced by Likhtman for describing the dy- namics of dense polymer melts. After reviewing the technical aspects associated with the implemen- tation of the model, we extend previous work in several directions. The dependence of the relaxation modulus with the slip link density and the slip link stiffness is reported. Then the nonlinear rheolog- ical properties of the model, for a particular set of parameters, are explored. Finally, we introduce excluded volume interactions in a mean field such as manner in order to describe inhomogeneous systems, and we apply this description to a simple nanocomposite model. With this extension, the slip link model appears as a simple and generic model of a polymer melt, that can be used as an alternative to molecular dynamics for coarse grained simulations of complex polymeric systems.

cond-mat.soft↗

arXiv2012

Thermal conductance at the interface between crystals using equilibrium and non-equilibrium molecular dynamics

In this article, we compare the results of non-equilibrium (NEMD) and equilibrium (EMD) molecular dynamics methods to compute the thermal conductance at the interface between solids. We propose to probe the thermal conductance using equilibrium simulations measuring the decay of the thermally induced energy fluctuations of each solid. We also show that NEMD and EMD give generally speaking inconsistent results for the thermal conductance: Green Kubo simulations probe the Landauer conductance between two solids which assumes phonons on both sides of the interface to be at equilibrium. On the other hand, we show that NEMD give access to the out-of-equilibrium interfacial conductance consistent with the interfacial flux describing phonon transport in each solid. The difference may be large and reaches typically a factor 5 for interfaces between usual semi-conductors. We analyze finite size effects for the two determinations of the interfacial thermal conductance, and show that the equilibrium simulations suffer from severe size effects as compared to NEMD. We also compare the predictions of the two above mentioned methods -EMD and NEMD- regarding the interfacial conductance of a series of mass mismatched Lennard-Jones solids. We show that the Kapitza conductance obtained with EMD can be well described using the classical diffuse mismatch model (DMM). On the other hand, NEMD simulations results are consistent with a out-of-equilibrium generalisation of the acoustic mismatch model (AMM). These considerations are important in rationalizing previous results obtained using molecular dynamics, and help in pinpointing the physical scattering mechanisms taking place at atomically perfect interfaces between solids, which is a prerequesite to understand interfacial heat transfer across real interfaces.

cond-mat.mes-hall↗