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Lydéric Bocquet

Publications and source records attributed to Lydéric Bocquet.

At least 19 recordsLinked to original sources

Fluctuation-induced ionic friction at solid-electrolyte interfaces

In this article, we explore how transport at a solid--electrolyte interface is affected by the internal fluctuations of the solid and quantify the role of solid excitations on ionic friction. Combining molecular dynamics simulations with theoretical modeling, we show that the presence of ions enhances the dynamical response of the electrolyte compared to pure water. This leads to an ionic contribution to the fluctuation-induced interfacial friction. We show that collective ionic modes dominate the dissipation, such that ionic friction arises from many-body effects rather than from individual drag forces. Furthermore, high-frequency molecular modes are found to be ion-specific, suggesting possible routes toward spectral separation of ions, with implications for desalination, filtration, and energy conversion.

cond-mat.soft↗

Fluctuation-induced and quantum effects in nanofluidic transport

The hydrodynamic wall has traditionally been considered a featureless object, whose only role is to provide a boundary for fluid flow. Yet, there is now ample evidence that at nanometer scales, liquid flows are sensitive to the wall's internal -- in particular, electronic -- degrees of freedom. Here, after reviewing the experimental evidence for nanoscale liquid-electron couplings, we present the theoretical advances that have allowed for their quantitative understanding. We discuss how a quantum description of the liquid-solid interface reveals the influence of electron dynamics on classical fluid transport, in the form of the fluctuation-induced quantum friction effect. Quantum friction is at the root of liquid-electron coupled transport phenomena, that may be combined into a hydro-electronic transport matrix. We present analytical formulas for the hydro-electronic transport coefficients, that allow for their quantitative estimation in practical cases; we further outline the potential consequences of coupled liquid-electron transport for the water-energy nexus. Fluctuation-induced and quantum effects at liquid-solid interfaces represent an emerging interface between fluid dynamics and condensed-matter physics, and a largely uncharted territory for both theory and experiment.

physics.flu-dyn↗

Diffusio-osmotic transport in nanochannels

In this chapter, I will enter into the roots of entropically-driven transport with a focus on diffusio-osmotic transport in nanochannels. Diffusio-osmosis is a subtle surface transport, originating in entropic driving forces occuring within the diffuse layers at solid boundaries. Specifying diffusio-osmosis to nanochannels may first look like a marginal refinement, yet it reveals that osmotic drivings can arise in channels and membranes without the prerequisite of semi-permeability, so that diffusio-osmosis extends the domain of existence of entropically driven transport. Osmosis and diffusio-osmosis are two faces of the same phenomenon, naturally embedded in an Onsager framework and quantified by local and global force balances. This perspective clarifies why nanochannels are privileged arenas where diffusio-osmosis and its consequence do flourish. Throughout the chapter, I discuss a set of conceptually relevant examples to show how diffusio-osmosis "pops up" in various situations: as enhanced diffusion, mechano-sensitivity, rectified osmotic flows and, ultimately, as a lever for osmotic energy conversion from single nanopores to membrane modules approaching industrial reality.

cond-mat.soft↗

Architecting mechanosensitive nanofluidic transport in graphite nanoslits

Mechanosensitive ion transport plays a central role in enabling living systems to perceive and adapt to their environment through the deformation of soft, embedded ion channels. In this work, we demonstrate that ion transport within a two-dimensional graphite nanoslit can be rationally engineered to achieve a bipolar, pressure-sensitive response without any structural deformation. The mechanosensitivity arises from the selective charging of one channel inlet, which acts as a reversible source of mobile charge carriers. These excess-ions can then be advected in or out of the channel by the pressure-driven water flow, thereby modulating the ionic conductance. This mechanism is captured through a comprehensive electrohydrodynamic model that analytically accounts for coupled diffusion, convection, surface transport, diffusio-osmosis, and interfacial slippage, both inside and outside the nanoslit. The theoretical framework quantitatively reproduces the experimental data, showing that a simple surface charge pattern can give rise to complex, pressure-dependent conductance. These findings reveal how rich nonlinear couplings at the nanoscale can be harnessed to design adaptive, bioinspired nanofluidic systems, exemplified here by ionic pressure sensors.

cond-mat.soft↗

Electron-electrolyte coupling in AC transport through nanofluidic channels

The transport properties of nanofluidic channels are usually studied under constant (DC) voltage or pressure driving. However, the frequency response under sinusoidal (AC) drivings offers rich insights into the time-dependent transport mechanisms. Inspired by recent electrochemical approaches, we investigate the couplings between ionic and electronic transport under AC driving. We show that conduction electrons of the channel walls participate in ionic current via capacitive electrochemical coupling, defining a critical frequency and length scale where electron-dominated conductivity emerges. We further analyze how electron-ion coupling modifies electro-osmotic flows, and demonstrate that fluctuation-induced momentum transfer between the electrolyte and wall electrons produces distinct AC transport signatures depending on the charge carrier polarity. Altogether, we establish a frequency-dependent transport matrix that couples ionic, electronic and hydrodynamic flows. These findings establish AC nanofluidic transport as a powerful probe of interfacial phenomena under confinement, and suggest new directions for engineering nanofluidic functionalities through electron-electrolyte coupling.

cond-mat.mes-hall↗

Combined effects of evaporation, sedimentation and solute crystallization on the dynamics of aerosol size distributions on multiple length and time scales

We investigate three aspects of aerosol-mediated air-borne viral infection mechanisms on different length and time scales. First, we address the evolution of the size distribution of a non-interacting ensemble of droplets that are subject to evaporation and sedimentation using a sharp droplet-air interface model. From the exact solution of the evolution equation we derive the viral load in the air and show that it depends sensitively on the relative humidity. Secondly, from Molecular Dynamics simulations we extract the molecular reflection coefficient of single water molecules from the air-water interface. This parameter determines the water condensation and evaporation rate at a liquid droplet surface and therefore the evaporation rate of aqueous droplets. We find the reflection of water to be negligible at room temperature but to rise significantly at elevated temperatures and for grazing incidence angles. Thirdly, we derive a thermodynamically consistent three-dimensional diffuse-interface model for solute-containing droplets that is formulated as a three-phase Cahn-Hilliard/Allen-Cahn system. By numerically solving the coupled system of equations, we explore representative scenarios that show that this model reproduces and generalizes features of the sharp-interface model. These interconnected studies on the dynamics of aerosol droplet evaporation are relevant in order to quantitatively assess the airborne infection risk under varying environmental conditions.

physics.flu-dyn↗

Hydrodynamic permeability of fluctuating porous membranes

In this paper we examine how porosity fluctuations affect the hydrodynamic permeability of a porous matrix or membrane. We introduce a fluctuating Darcy model, which couples the Navier-Stokes equation to the space- and time-dependent porosity fluctuations via a Darcy friction term. Using a perturbative approach, a Dyson equation for hydrodynamic fluctuations is derived and solved to express the permeability in terms of the matrix fluctuation spectrum. Surprisingly, the model reveals strong modifications of the fluid permeability in fluctuating matrices compared to static ones. Applications to various matrix excitation models - breathing matrix, phonons, active forcing - highlight the significant influence of matrix fluctuations on fluid transport, offering insights for optimizing membrane design for separation applications.

cond-mat.soft↗

Ionic association and Wien effect in 2D confined electrolytes

Recent experimental advances in nanofluidics have allowed to explore ion transport across molecular-scale pores, in particular for iontronic applications. Two dimensional nanochannels -- in which a single molecular layer of electrolyte is confined between solid walls -- constitute a unique platform to investigate fluid and ion transport in extreme confinement, highlighting unconventional transport properties. In this work, we study ionic association in 2D nanochannels, and its consequences on non-linear ionic transport, using both molecular dynamics simulations and analytical theory. We show that under sufficient confinement, ions assemble into pairs or larger clusters in a process analogous to a Kosterlitz-Thouless transition, here modified by the dielectric confinement. We further show that the breaking of pairs results in an electric-field dependent conduction, a mechanism usually known as the second Wien effect. However the 2D nature of the system results in non-universal, temperature-dependent, scaling of the conductivity with electric field, leading to ionic coulomb blockade in some regimes. A 2D generalization of the Onsager theory fully accounts for the non-linear transport. These results suggest ways to exploit electrostatic interactions between ions to build new nanofluidic devices.

cond-mat.soft↗

Momentum tunnelling between nanoscale liquid flows

The world of nanoscales in fluidics is the frontier where the continuum of fluid mechanics meets the atomic, and even quantum, nature of matter. While water dynamics remains largely classical under extreme confinement, several experiments have recently reported coupling between water transport and the electronic degrees of freedom of the confining materials. This avenue prompts us to reconsider nanoscale hydrodynamic flows under the perspective of interacting excitations, akin to condensed matter frameworks. Here we show, using a combination of many-body theory and molecular simulations, that the flow of a liquid can induce the flow of another liquid behind a separating wall, at odds with the prediction of continuum hydrodynamics. We further show that the range of this 'flow tunnelling' can be tuned through the solid's electronic excitations, with a maximum occurring when these are at resonance with the liquid's charge density fluctuations. Flow tunnelling is expected to play a role in global transport across nanoscale fluidic networks, such as lamellar graphene oxide or MXene membranes. It further suggests exploiting the electronic properties of the confining walls for manipulating liquids via their dielectric spectra, beyond the nature and characteristics of individual molecules.

cond-mat.mes-hall↗

Hydroelectric energy conversion of waste flows through hydroelectronic drag

Hydraulic energy is a key component of the global energy mix, yet there exists no practical way of harvesting it at small scales, from flows at low Reynolds number. This has triggered the search for alternative hydroelectric conversion methodologies, leading to unconventional proposals based on droplet triboelectricity, water evaporation, osmotic energy or flow-induced ionic Coulomb drag. Yet, these approaches systematically rely on ions as intermediate charge carriers, limiting the achievable power density. Here, we predict that the kinetic energy of small-scale "waste" flows can be directly and efficiently converted into electricity thanks to the hydro-electronic drag effect, by which an ion-free liquid induces an electronic current in the solid wall along which it flows. This effect originates in the fluctuation-induced coupling between fluid motion and electron transport. We develop a non-equilibrium thermodynamic formalism to assess the efficiency of such hydroelectric energy conversion, dubbed hydronic energy. We find that hydronic energy conversion is analogous to thermoelectricity, with the efficiency being controlled by a dimensionless figure of merit. However, in contrast to its thermoelectric analogue, this figure of merit combines independently tunable parameters of the solid and the liquid, and can thus significantly exceed unity. Our findings suggest new strategies for blue energy harvesting without electrochemistry, and for waste flow mitigation in membrane-based filtration processes.

physics.flu-dyn↗

Anomalous friction of supercooled glycerol on mica

The fundamental understanding of friction of liquids on solid surfaces remains one of the key knowledge gaps in the transport of fluids. While the standard perspective emphasizes the role of wettability and commensurability, recent works have unveiled the crucial role of the solid's internal excitations, whether electronic or phononic, on liquid-solid dissipation. In this work, we take advantage of the considerable variation of the molecular timescales of supercooled glycerol under mild change of temperature, in order to explore how friction depends on the liquid's molecular dynamics. Using a dedicated tuning-fork-based AFM to measure the hydrodynamic slippage of glycerol on mica, we report a 2-order of magnitude increase of the slip length with decreasing temperature by only 30°C. However the solid-liquid friction coefficient is found to be a non monotonous function of the fluid molecular relaxation rate, fα, at odd with an expected Arrhenius behavior. In particular, the linear increase of friction with the liquid molecular rate measured at high temperature cannot be accounted for by existing modelling. We show that this unconventional and non-arrhenian friction is consistent with a contribution of the solid's phonons to the liquid-solid friction. This dynamical friction opens new perspectives to control hydrodynamic flows by properly engineering phononic and electronic excitation spectra in channel walls.

cond-mat.soft↗

Drastic reduction of dynamic liquid-solid friction in supercooled glycerol

This study addresses the influence of internal liquid dynamics on liquid-solid friction. Taking advantage of the wide range of relaxation timescales in supercooled liquids, we use a tuning-fork-based AFM to measure the slippage of supercooled glycerol on mica at 30 kHz. We report a 2-order of magnitude increase of slippage with decreasing temperature by only 30°C. More importantly, as the bulk liquid dynamics are slowed with decreasing temperature, we report a sharp drop of the interfacial friction coefficient in contrast with the usual assumption of thermally activated interfacial dynamics. To rationalize this original behavior, we account for the contribution of solid fluctuations to liquid friction. We show that a minimalistic single phonon-branch model of the mica surface yields semi-quantitative agreement with our measurements. In this picture, the liquid's relaxation rate is the tuning knob between two friction regimes where the wall is seen either as a static corrugated potential or as a thermally fluctuating surface. Remarkably, this study bridges soft and hard condensed matter: hydrodynamic flow controlled by the solid's dynamical modes.

cond-mat.soft↗

Unified non-equilibrium simulation methodology for flow through nanoporous carbon membrane

The emergence of new nanoporous materials, based e.g. on 2D materials, offers new avenues for water filtration and energy. There is accordingly a need to investigate the molecular mechanisms at the root of the advanced performances of these systems in terms of nanofluidic and ionic transport. In this work, we introduce a novel unified methodology for Non-Equilibrium classical Molecular Dynamic simulations (NEMD), allowing to apply likewise pressure, chemical potential and voltage drops across nanoporous membranes and quantifying the resulting observables characterizing confined liquid transport under such external stimuli. We apply the NEMD methodology to study a new type of synthetic Carbon NanoMembranes (CNM), which have recently shown outstanding performances for desalination, keeping high water permeability while maintaining full salt rejection. The high water permeance of CNM, as measured experimentally, is shown to originate in prominent entrance effects associated with negligible friction inside the nanopore. Beyond, our methodology allows to fully calculate the symmetric transport matrix and the cross-phenomena such as electro-osmosis, diffusio-osmosis, streaming currents, etc. In particular, we predict a large diffusio-osmotic current across the CNM pore under concentration gradient, despite the absence of surface charges. This suggests that CNMs are outstanding candidates as alternative, scalable membranes for osmotic energy harvesting.

cond-mat.mes-hall↗

Collective modes and quantum effects in two-dimensional nanofluidic channels

Nanoscale fluid transport is typically pictured in terms of atomic-scale dynamics, as is natural in the real-space framework of molecular simulations. An alternative Fourier-space picture, that involves the collective charge fluctuation modes of both the liquid and the confining wall, has recently been successful at predicting new nanofluidic phenomena such as quantum friction and near-field heat transfer, that rely on the coupling of those fluctuations. Here, we study the charge fluctuation modes of a two-dimensional (planar) nanofluidic channel. Introducing confined response functions that generalize the notion of surface response function, we show that the channel walls exhibit coupled plasmon modes as soon as the confinement is comparable to the plasmon wavelength. Conversely, the water fluctuations remain remarkably bulk-like, with significant confinement effects arising only when the wall spacing is reduced to 7 A. We apply the confined response formalism to predict the dependence of the solid-water quantum friction and thermal boundary conductance on channel width for model channel wall materials. Our results provide a general framework for Coulomb interactions of fluctuating matter in nanoscale confinement.

cond-mat.mes-hall↗

Disentangling $1/f$ noise from confined ion dynamics

Ion transport through biological and solid-state nanochannels is known to be a highly noisy process. The power spectrum of current fluctuations is empirically known to scale like the inverse of frequency, following the long-standing yet poorly understood Hooge's law. Here, we report measurements of current fluctuations across nanometer-scale two-dimensional channels with different surface properties. The structure of fluctuations is found to depend on channel's material. While in pristine channels current fluctuations scale like $1/f^{1+a}$ with $a = 0 - 0.5$, the noise power spectrum of activated graphite channels displays different regimes depending on frequency. Based on these observations, we develop a theoretical formalism directly linking ion dynamics and current fluctuations. We predict that the noise power spectrum take the form $1/f \times S_\text{channel}(f)$, where $1/f$ fluctuations emerge in fluidic reservoirs on both sides of the channel and $S_\text{channel}$ describes fluctuations inside it. Deviations to Hooge's law thus allow direct access to the ion transport dynamics of the channel -- explaining the entire phenomenology observed in experiments on 2D nanochannels. Our results demonstrate how current fluctuations can be used to characterize nanoscale ion dynamics.

cond-mat.soft↗

Nanofluidics at the crossroads

Nanofluidics, the field interested in flows at the smallest scales, has grown at a fast pace, reaching an ever finer control offluidic and ionic transport at the molecular level. Still, artificial pores are far from reaching the wealth of functionalities of biological channels that regulate sensory detection, biological transport and neurostransmission - all while operating at energies comparable to thermal noise. Here, we argue that artificial ionic machinescan be designed by harnessing the entire wealth of phenomena available at the nanoscales and exploiting techniques developped in various fields of physics. As they are generally based on solid-state nanopores, rather than soft membranes and proteins, they should in particular aim at taking advantage of their specific properties such as their electronic structure or their ability to interact with light. These observations call for the design of new ways of probing nanofluidic systems. Nanofluidics is now at the crossroads, there are new avenues to build complex ionic machines and this may allow to develop new functionalities inspired by Nature.

cond-mat.soft↗

Quantum feedback at the solid-liquid interface: flow-induced electronic current and its negative contribution to friction

An electronic current driven through a conductor can induce a current in another conductor through the famous Coulomb drag effect. Similar phenomena have been reported at the interface between a moving fluid and a conductor, but their interpretation has remained elusive. Here, we develop a quantum-mechanical theory of the intertwined fluid and electronic flows, taking advantage of the non-equilibrium Keldysh framework. We predict that a globally neutral liquid can generate an electronic current in the solid wall along which it flows. This hydrodynamic Coulomb drag originates from both the Coulomb interactions between the liquid's charge fluctuations and the solid's charge carriers, and the liquid-electron interaction mediated by the solid's phonons. We derive explicitly the Coulomb drag current in terms of the solid's electronic and phononic properties, as well as the liquid's dielectric response, a result which quantitatively agrees with recent experiments at the liquid-graphene interface. Furthermore, we show that the current generation counteracts momentum transfer from the liquid to the solid, leading to a reduction of the hydrodynamic friction coefficient through a quantum feedback mechanism. Our results provide a roadmap for controlling nanoscale liquid flows at the quantum level, and suggest strategies for designing materials with low hydrodynamic friction.

cond-mat.mes-hall↗

Strong electronic winds blowing under liquid flows on carbon surfaces

The interface between a liquid and a solid is the location of plethora of intrincate mechanisms at the nanoscale, at the root of their specific emerging properties in natural processes or technological applications. However, while the structural properties and chemistry of interfaces have been intensively explored, the effect of the solid-state electronic transport at the fluid interface has been broadly overlooked up to now. It has been reported that water flowing against carbon-based nanomaterials, such as carbon nanotubes or graphene sheets, does induce electronic currents, but the mechanism at stake remains controversial. Here, we unveil the molecular mechanisms underlying the hydro-electronic couplings by investigating the electronic conversion under flow at the nanoscale. We use a tuning fork-Atomic Force Microscope (AFM) to deposit and displace a micrometric droplet of both ionic and non-ionic liquids on a multilayer graphene sample, while recording the electrical current across the carbon flake. We report measurements of an oscillation-induced current which is several orders of magnitude larger than previously reported for water on carbon , and further boosted by the presence of surface wrinkles on the carbon layer. Our results point to a peculiar momentum transfer mechanism between fluid molecules and charge carriers in the carbon walls mediated by phonon excitations in the solid. Our findings pave the way for active control of fluid transfer at the nanoscale by harnessing the complex interplay between collective excitations in the solid and the molecules in the fluid.

cond-mat.mes-hall↗