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Thomas Salez

Publications and source records attributed to Thomas Salez.

At least 19 recordsLinked to original sources

Broadband molecular dynamics simulation of fluid inertial effects in confined Brownian motion

Hydrodynamic memory governs Brownian motion over a broad range of timescales, from acoustic wave propagation at short times to diffusive relaxation at long times. While confinement-induced corrections to Brownian diffusion are well established, how confinement modifies the full hydrodynamic response remains less explored. In this Letter, we use molecular-dynamics simulations of a neutrally buoyant colloidal particle in an explicit solvent to resolve the velocity autocorrelation function across a broad hydrodynamic spectrum. In the bulk, the simulations recover compressibility, added mass, the hydrodynamic long-time tail, and Stokes-Einstein diffusion without adjustable parameters. Near a rigid wall, the velocity correlations become anisotropic, their algebraic tails are modified, and the diffusion coefficients are reduced. Most importantly, the short-time dynamics reveals a pronounced enhancement of the effective added mass as the wall is approached. As such, the velocity autocorrelation function appears as a central quantity to bridge the zero-frequency mobility and the high-frequency inertial behaviour of a confined Brownian particle.

cond-mat.soft

Quantitative measurement of fluid inertial effects in confined Brownian motion

The hydrodynamic response of Brownian particles in liquids is fundamentally altered by inertial forces arising from unsteady momentum transport in the surrounding fluid. These forces are of two distinct types\,: the added mass and the history effect. While both are well understood in bulk and weakly-confined geometries, under deterministic driving, their respective behaviours under strong confinement and thermal fluctuations remain scarcely addressed, unclear and often entangled together. The goal of the present study is thus to fill this fundamental gap. The behaviours of the two distinct inertial contributions are quantitatively investigated in the vicinity of a flat, rigid wall, using a combination of broadrange thermal colloidal-probe atomic-force-microscopy experiments, advanced numerical simulations and theory. The separation of the added-mass and history-force contributions is achieved through their different frequency-scaling signatures within the measured high-resolution thermal spectra. Our results establish a complete picture of Brownian motion at interfaces, in the lubrication regime, with direct relevance to nanofluidics and interfacial biophysics.

cond-mat.soft

Nanostructure of PEGDA-PEG hydrogel membranes and how it controls their permeability

The spacial heterogeneity of hydrogels composed of PEGDA and added polymer chains is expected to play a crucial role on their transport properties which can be exploited in filtration or tissue engineering. However little is known about the arrangement of the polymer chains in the matrix and the length scales of these heterogeneities. Here we combine solid-state NMR and Small Angle Neutron Scattering to unravel the structure and dynamics of PEGDA hydrogels containing added PEG chains of various concentrations. Our results show that the samples present heterogeneities in both the PEGDA and PEG concentrations and suggest that the PEG chains entangle with the PEGDA network. When plotting the sample permeability, K, as a function the specific surface of the PEGDA heterogeneities we obtain a master curve, showing that the heterogeneity of the PEGDA matrix controls the permeability of the sample. Moreover the scaling K ___ V/S suggests a structure composed of facetted PEGDA/PEG heterogeneities separated by a network of aqueous thin and flattened films in which the water can permeate.

cond-mat.soft

Linear poroelastic response of thin permeable gel films

When a hydrophilic and deformable porous material is immersed in a bath, it may absorb the solvent and expand by several times its volume, thus forming a highly soft and porous hydrogel. A stress applied on the soft hydrogel surface deforms it and forces the absorbed solvent to move by flowing through the network of pores. This coupled phenomenon sets the framework of poroelasticity. Moreover, polymeric gels are often used in ultra-thin coatings to tune surface properties. Together with the characteristic poroelastic coupling, this thinness challenges the modelling of their response. In this article, we derive the point-force mechanical response of a thin, permeable and poroelastic layer bounded to a rigid substrate. We show that the gel surface is only deformed around the indentation point, within a radius on the order of the layer thickness. The obtained Green's function can be directly used to predict the space- and time-dependent surface deformation of the gel. Our findings are relevant for a broad range of applications, such as indentation experiments on swollen gels, thin membranes or soft and living systems, as well as lubrication problems involving a soft and porous wall, for instance in microfluidics.

cond-mat.soft

Electrohydrodynamic lubrication theory for an immersed cylinder moving near wall

The free motion of charged colloids within ionic solutions and in the vicinity of charged boundaries, is a phenomenon that occurs in various natural, biological and industrial settings. Here, we develop an electrohydrodynamic lubrication theoretical framework, in order to characterize such a motion in the case of an infinite rigid cylinder near a rigid wall. Combining hydrodynamic lubrication theory, Debye-H\''uckel electrostatics, and Nernst-Planck electrokinetics, we derive the three coupled equations of motion for the normal, longitudinal and rotational degrees of freedom of the cylinder, which are then investigated numerically and through asymptotic analysis. Our results reveal complex behaviours, beyond existing asymptotic electroviscous-lift expressions, and extend the classical Faxen-Brenner-like mobility matrix when surface charges and dissolved ions are incorporated.

cond-mat.soft

Polymeric Solvents Control Swelling-Induced Surface Creasing

Surface creasing in swelling polymer gels is commonly attributed to compressive strain or interlayer mismatch, yet its general control remains unclear. Here we show that solvent polymerization degree $N_{\rm s}$ provides an independent control parameter for crease onset in surface-bound polydimethylsiloxane gels swollen by silicone oils. Despite nearly identical swelling kinetics and through-thickness solvent concentration profiles, we observe a transition from creased to stable surfaces with increasing $N_{\rm s}$. A theory coupling swelling thermodynamics and mechanical stability reveals that polymeric solvents reduce the mixing entropy and thereby modify the osmotic pressure, allowing $N_{\rm s}$ to tune separately the equilibrium swelling and the crease threshold. This framework captures the stability boundary across solvent polymerization degree and network elasticity. These results identify polymeric solvents as active thermodynamic-mechanical regulators of swelling-induced surface.

cond-mat.soft

Taylor dispersion in a soft channel

Diffusion of a solute along a channel is enhanced by hydrodynamic flow, a phenomenon known as Taylor dispersion. In microfluidic applications, the compliance of the channel boundaries modifies the hydrodynamic flow and thus solutal transport. Here, we develop the theory of solutal dispersion in a soft, axisymmetric channel where the channel walls respond to the hydrodynamic pressure through a Winkler response. By deriving the modified macro-transport equation for the solutal concentration dynamics based on multiple-time-scale analysis, we explore the influence of softness on solutal transport for steady and pulsatile configurations. Our main finding is that softness enhances the effective advection velocity and dispersion coefficient, which might have practical implication in biology and microfluidic technology.

cond-mat.soft

A label-free method to quantify early-stage amyloid aggregation via intrinsic phenylalanine fluorescence

The aggregation of amyloid-forming peptides is a dynamic, complex process that underlies their diverse biological activities, from physiological functions to disease-associated dysfunctions. While the structure of fibrillar end-products is well-characterized for most amyloids, the heterogeneous and often transient oligomers, likely key in cytotoxicity, remain poorly investigated, especially for peptides with low-yield aromatic residues. Here, by exploiting and developing flow induced dispersion analysis in both peak and front modes, we demonstrate that intrinsic phenylalanine fluorescence can be harnessed to quantify the conversion of diffusing monomers into non-diffusing oligomers and fibrils. This approach is validated using PSM$\alpha$3, a tryptophan- and tyrosine-free peptide from S. aureus, known for its fast amyloid fibrillation and key roles in bacterial virulence. We indeed characterize its low-molecular-weight oligomers, and size evolution from 2 to 10 nm over time. Importantly, to further validate the robustness of our front-mode approach, we apply it to hIAPP, a tyrosine-containing, tryptophan-free peptide, with critical outcome in type 2 diabetes. Our results overcome the limitations of traditional biochemical and biophysical amyloid assays by extending analysis from large oligomers and fibrils to small heterogeneous oligomers, under near-physiological conditions. This study thus offers a new analytical framework, thereby filling a critical gap in amyloid research, to probe the early stages of aggregation, key in the design of alternative therapeutics for amyloid-diseases.

cond-mat.soft

Suppressed Rupture of Thin Metal Films via van der Waals Epitaxy

Ultrathin metal films exhibit liquid-like instabilities, rupturing via surface diffusion far below their melting points. This behavior constrains thermal budgets for advanced integrated circuits and emerging 2D-crystal devices. Here, we demonstrate that these instabilities can be fundamentally suppressed using graphene as a van der Waals (vdW) template. While conventional 20-nm-thick gold films break up into islands below 300 {\textdegree}C, templated films not only remain stable but also become structurally refined after annealing above 600 {\textdegree}C. This exceptional stability stems from a vdW-mediated crystallographic texture that reorganizes grain boundaries into a mechanically robust network. This mechanism significantly widens the processing window for nanoscale interconnects and enables high-temperature integration of metals with 2D-crystal technologies.

cond-mat.soft

Inferring intraciliary dynamics from the gliding motility of Chlamydomonas reinhardtii

The unicellular microalga Chlamydomonas reinhardtii is widely recognized as a premier model living microswimmer for physicists and biophysicists. However, the interest around C. reinhardtii goes beyond its swimming capabilities. In fact, light can drastically alter its behavior: under blue illumination, the cell attaches to a nearby surface and intermittently glides on it. Such a gliding motility is powered by molecular-motor proteins operating on the cell's cilia, and the related machinery has established the cell as a prime reference for the study of intraciliary-transport mechanisms. This is what we focus on in the present work, by combining in-line holographic microscopy -which leads to unprecedented spatial and temporal resolutions on the gliding dynamics -and statistical inference. We show that, while gliding, the cells exhibit anomalous-diffusive features, including Lorentzian-like distributions of displacements, which are reminiscent of enhanced search strategies. The latter may be exploited by the cells to facilitate colony formation, or, more broadly, by organisms possessing an intraciliary-transport machinery for the transport of cargo molecules and signaling. Furthermore, gliding trajectories, by being intermittent, are valid candidates to infer forces at the molecular-motor scale that are necessary for the cells to move, or symetrically, to transport cargo molecules. We report a gliding threshold of about 20 pN, compatible with the activity of single molecular motors.

cond-mat.soft

First-passage statistics of confined colloids

The encounter of diffusing entities underlies a wide range of natural phenomena. The dynamics of these first-passage dynamics are strongly influenced by confining geometries. Confinement modifies microscopic diffusion through conservative and hydrodynamic interactions, making it essential for realistic modeling. In this Letter, we investigate how confinement affects the first-passage statistics of a diffusing particle. Using \textit{state-of-the-art} holographic microscopy combined with advanced statistical inference, we probe this motion with nanometric precision. Our experimental and numerical results show that confinement can either hinder or enhance first-passage kinetics, depending on the spatial direction. In particular, wall-normal target finding is accelerated by confinement-induced non-Gaussian displacement statistics, which increases the probability of rare, large displacements, with implications for confined chemical reactions and biological \textit{winners-take-all} processes near boundaries.

cond-mat.soft

pH-dependent interfacial rheology of polymer membranes assembled at liquid-liquid interfaces using hydrogen bonds

Self-assembly of polymers at liquid interfaces using non-covalent interactions has emerged as a promising technique to reversibly produce self-healing membranes. Besides the assembly process, it is also crucial to control the mechanical properties of these membranes. Here, we measure the interfacial rheological properties of PMAA-PPO (polymethacrylic acid - polypropylene oxide) polymer membranes assembled using hydrogen bonds at the interface between water and a polar oil, Mygliol. Varying the pH enables us to modify the degree of ionization of the PMAA chains, and hence their ability to establish hydrogen interactions with PPO. Frequency sweeps of the interfacial layers show a crossover between a viscous regime at low frequencies and an elastic regime at high frequencies. The crossover elastic modulus, measured one hour after the two phases were put into contact, decreases by a half over the pH range investigated, which can be accounted for by a decrease of the layer thickness as pH increases. Furthermore, we find that the crossover frequency varies exponentially with the degree of ionization of PMAA. To account for these observations, we propose a simple picture where the short PPO chains behave as non-covalent cross-linkers that bridge several PMAA chains. The dissociation rate and hence the crossover frequency are controlled by the number of PO units per PPO chain involved in the hydrogen bonds.

cond-mat.soft

Enhanced dispersion of active microswimmers in confined flows

In the presence of a laminar shear flow, the diffusion of passive colloidal particles is enhanced in the direction parallel to the flow. This classical phenomenon is known as Taylor-Aris dispersion. Besides, microorganisms, such as active microswimmers, exhibit an effective diffusive behavior at long times. Combining the two ingredients above, a natural question then emerges on how the effective diffusion of active microswimmers is altered in shear flows -- a widespread situation in natural environments with practical implications, \textit{e.g.} regarding biofilm formation. In this Letter, we investigate the motility and dispersion of \textit{Chlamydomonas reinhardtii} microalgae, within a rectangular microfluidic channel subjected to a sinusoidal Poiseuille flow. Using high-resolution optical microscopy and a particle-tracking algorithm, we reconstruct individual trajectories in various flow conditions and statistically analyze them through moment theory and sliding windowed demodulation. We find that the velocity fluctuations and the dispersion coefficient increase as the flow amplitude is increased, with only weak dependencies on the flow periodicity. Importantly, our results demonstrate that the generalization of Taylor-Aris law to active particles is valid.

cond-mat.stat-mech

Brownian motion near a soft surface

Brownian motion near soft surfaces is a situation widely encountered in nanoscale and biological physics. However, a complete theoretical description is lacking to date. Here, we theoretically investigate the dynamics of a two-dimensional colloid in an arbitrary external potential and near a soft surface. The latter is minimally modelled by a Winkler's foundation, and we restrict the study to the colloidal motion in the direction perpendicular to the surface. We start from deterministic hydrodynamic considerations, by invoking the already-established leading-order soft-lubrication forces acting on the particle. Importantly, a negative softness-induced and position-dependent added mass is identified. We then incorporate thermal fluctuations in the description. In particular, an effective Hamiltonian formulation is introduced and a temperature-dependent generalized potential is constructed in order to ensure equilibrium properties for the colloidal position. From these considerations and the Fokker-Planck equation, we then derive the relevant Langevin equation, which self-consistently allows to recover the deterministic equation of motion at zero temperature. Interestingly, besides an expected multiplicative-noise feature, the noise correlator appears to be modified by the surface softness. Moreover, a softness-induced temperature-dependent spurious drift term has to be incorporated within the Ito prescription. Finally, using numerical simulations with various initial conditions and parameter values, we statistically analyze the trajectories of the particle when placed within a harmonic trap and in presence of the soft surface. This allows us to: i) quantify further the influence of surface softness, through the added mass, which enhances the velocity fluctuations; and ii) show that intermediate-time diffusion is unaffected by softness, within the assumptions of the model.

cond-mat.soft

Surface mobility of a glass-forming polymer in an ionic liquid

The free surface of glassy polymers exhibits enhanced segmental dynamics compared to the bulk, forming a liquid-like layer that lowers the glass transition temperature (Tg) in nanometersized polymer samples. Recent studies have shown that immersing polymers in ionic liquids can suppress this enhanced surface dynamics. To investigate how ionic liquids influence polymer dynamics near the ionic-liquid-polymer interface, we measure the surface leveling of nanometersized stepped polystyrene films immersed in ionic liquids, and compared the results to the case of films in vacuum. Our results reveal that ionic liquids significantly slow the leveling process both above and below Tg. However, our results indicate that the liquid-like surface layer below Tg does exist in ionic liquids. Numerical solutions of the thin-film equation, incorporating appropriate boundary conditions, show that the surface mobility of PS films in ionic liquids can match that of PS films in vacuum. Thus, while ionic liquids alter the polymer flow process, they do not eliminate the dynamical heterogeneity inherent to glassy polymers.

cond-mat.soft

Enhanced diffusion over a periodic trap by hydrodynamic coupling to an elastic mode

In many physical systems, degrees of freedom are coupled \emph{via} hydrodynamic forces, even in the absence of Hamiltonian interactions. A particularly important and widespread example concerns the transport of microscopic particles in fluids near deformable boundaries. In such a situation, the influence of elastohydrodynamic couplings on Brownian motion remains to be understood. Unfortunately, the temporal and spatial scales associated with the thermal fluctuations of usual surfaces are often so small that their deformations are difficult to monitor experimentally, together with the much slower and larger particle motion at stake. Here, we propose a minimal model describing the hydrodynamic coupling of a colloidal particle to a fluctuating elastic mode, in presence of an external periodic potential. We demonstrate that the late-time diffusion coefficient of the particle increases with the compliance of the elastic mode. Remarkably, our results reveal that, and quantify how: i) spontaneous microscopic transport in complex environnements can be affected by soft boundaries -- a situation with numerous practical implications in nanoscale and biological physics; ii) the effects of fast and tiny surface deformations are imprinted over the long-term and large-distance colloidal mobility -- and are hence measurable in practice.

cond-mat.soft

The Soft-Membrane Surface Forces Apparatus

Compliant walls are widespread in biological and engineering systems. Because of their singular nature, adapted tools are required to accurately study their rheological properties as well as the consequences of the latter within a given mechanical setting. Because of their slender nature, membranes can be considered as prototypical examples of highly compliant boundaries. In this study, we describe a modified Surface Forces Apparatus (SFA) developed to measure the forces acting on a compliant membrane by measuring its deformation field. We discuss how such a device can be used to characterize the rheology of suspended membranes and accurately measure the electrostatic interactions between a polarized membrane and a spherical electrode, without the need of an external measurement spring.

cond-mat.soft

Bidirectional Mamba state-space model for anomalous diffusion

Characterizing anomalous diffusion is crucial in order to understand the evolution of complex stochastic systems, from molecular interactions to cellular dynamics. In this work, we characterize the performances regarding such a task of Bi-Mamba, a novel state-space deep-learning architecture articulated with a bidirectional scan mechanism. Our implementation is tested on the AnDi-2 challenge datasets among others. Designed for regression tasks, the Bi-Mamba architecture infers efficiently the effective diffusion coefficient and anomalous exponent from single, short trajectories. As such, our results indicate the potential practical use of the Bi-Mamba architecture for anomalousdiffusion characterization.

cond-mat.soft