arXiv subjects

Thierry Charitat

Publications and source records attributed to Thierry Charitat.

12 recordsLinked to original sources

arXiv2025

The role of confined water in the emergence of electrostatic strong coupling as revealed by nanoseparated charged lipid layers

This study investigates the interplay between Strong Coupling (SC) attraction and hydration repulsion in nanoconfined water between like-charged phospholipid layers. It challenges the assumption that SC attraction requires multivalent counterions by showing that hydration water can enhance electrostatic interactions. We combine reflectivities with numerical simulations to analyze supported phospholipid layers under different relative humidity and surface charge densities. X-ray fluorescence demonstrates that we can control the valence of the associated counterions. Experimental measurement of the water thickness, combined with precise determination of charged surface positions by numerical simulations, enable us to compare our experiments with a theoretical model. It shows that charge-screening by hydration water induces SC attraction, even at moderate surface charge densities with monovalent counterions. Furthermore, hydration repulsion is stronger for DPPS compared to DPPC. These findings offer insights into the forces that control interactions between phospholipid layers and have important implications for biological and colloidal systems.

cond-mat.soft↗

arXiv2025

Dielectric permittivity of water confined in stacks of charged lipid layers: extracting profiles from molecular dynamics simulations using a modified Poisson-Boltzmann equation

Most organic and inorganic surfaces (e.g., glass, nucleic acids or lipid membranes) become charged in aqueous solutions. The resulting ionic distribution induces effective interactions between the charged surfaces. Stacks of like-charged lipid bilayers immersed in multivalent ion solutions exhibit strong coupling (SC) effects, where ion correlations cause counter-intuitive membrane attraction. A similar attraction observed with monovalent ions is explained by SC theory through reduced dielectric permittivity under confinement. To explore this phenomenon, we propose a modified Poisson-Boltzmann (mPB) model with spatially varying dielectric permittivity and explicit Born solvation energy for ions. We use the model to investigate the dielectric permittivity profile of confined water in molecular dynamics simulations of charged lipid layers stacks at varying hydration levels, and compare the results with alternative computational methods. The model captures a sharp decrease in permittivity upon dehydration, converging to a plateau value that we attribute to lipid headgroups. The generic nature of the mPB framework allows application to other systems, such as other biological interfaces or solid walls, provided ions follow Boltzmann statistics. Finally, the increase of the area per lipid in our tension-free simulations of the fluid membranes hints that the permittivity decrease upon dehydration is concomitant with an intermembrane attraction.

cond-mat.soft↗

arXiv2022

Perturbing the catenoid: stability and mechanical properties of non-axisymmetric minimal surfaces

Minimal surface problems arise naturally in many soft matter systems whose free energies are dominated by surface or interface energies. Of particular interest are the shapes, stability and mechanical stresses of minimal surfaces spanning specific geometric boundaries. The "catenoid" is the best-known example where an analytical solution is known which describes the form and stability of a minimal surface held between two parallel, concentric circular frames. Here we extend this problem to non-axisymmetric, parallel frame shapes of different orientations, by developing a perturbation approach around the known catenoid solution. We show that the predictions of the perturbation theory are in good agreement with experiments on soap films and finite element simulations (Surface Evolver). Combining theory, experiment and simulation, we analyse in depth how the shapes, stability and mechanical properties of the minimal surfaces depend on the type and orientation of elliptical and three-leaf clover shaped frames. In the limit of perfectly aligned non-axisymmetric frames, our predictions show excellent agreement with a recent theory established by Alimov et al (M. M. Alimov, A. V. Bazilevsky and K. G. Kornev, Physics of Fluids, 2021, 33, 052104). Moreover, we put in evidence the intriguing capacity of minimal surfaces between non-axisymmetric frames to transmit a mechanical torque despite being completely liquid. These forces could be interesting to exploit for mechanical self-assembly of soft matter systems or as highly sensitive force captors.

cond-mat.soft↗

arXiv2020

Counter-rotation of magnetic beads in spinning fields

A magnetized bead in a magnetic field seeks to minimize its magnetic free energy by aligning its magnetic moment with the field direction and by moving towards the maximum of the field's intensity. However, when the bead is coupled to a substrate it is forced to roll. The two otherwise independent degrees of freedom, translation and rotation, become tightly coupled giving rise to subtle and often counterintuitive effects. Here we investigate one such, easily reproducible, yet stunning effect : A neodymium bead placed on top of a laboratory magnetic stirrer. When the stirrer's magnet spins at slow rates the bead naturally follows the field. However, surprisingly, at high spinning rates the bead suddenly inverts its direction and runs, to the surprise of the observer, in the opposite direction, against the driving field direction.This effect, experimentally investigated in [J.Magn.Magn.Matter, 476, 376-381, (2019)], is here comprehensively studied, with numerical simulations and a theoretical approach complementing experimental observations.

physics.class-ph↗

arXiv2019

Attractive Interaction between Fully Charged Lipid Bilayers in a Strongly-Confined Geometry

We investigate the interaction between highly charged lipid bilayers in the presence of monovalent counterions. Neutron and X-ray reflectivity experiments show that the water layer between like-charged bilayers is thinner than for zwitterionic lipids, demonstrating the existence of counterintuitive electrostatic attractive interaction between bilayers. Such attraction can be explained by taking into account the correlations between counterions within the Strong Coupling limit, which falls beyond the classical Poisson-Boltzmann theory of electrostatics. Our results show the limit of the Strong Coupling continuous theory in a highly confined geometry and are in agreement with a decrease in the water dielectric constant due to a surface charge-induced orientation of water molecules.

cond-mat.soft↗

arXiv2019

The role of shape disorder in the collective behaviour of aligned fibrous matter

We study the compression of bundles of aligned macroscopic fibers with intrinsic shape disorder, as found in human hair and in many other natural and man-made systems. We show by a combination of experiments, numerical simulations and theory how the statistical properties of the shapes of the fibers control the collective mechanical behaviour of the bundles. This work paves the way for designing aligned fibrous matter with pre-required properties from large numbers of individual strands of selected geometry and rigidity.

cond-mat.soft↗

arXiv2016

Worm-like instability of a vibrated sessile drop

We study the effects of vertical sinusoidal vibrations on a liquid droplet with a low surface tension (ethanol) deposited on a solid substrate. In a precise range of amplitudes and frequencies, the drop exhibits a dramatic worm-like shape instability with a strong symmetry breaking, comparable to the one observed by Pucci et al. (Phys. Rev. Lett., 106 (2011) 024503) on a vibrated floating lens. However, the geometry of our system is much simpler since it does not involve the oscillation and deformation of a liquid-liquid-air contact line. We show that the Faraday waves appearing on the surface of the droplet control its shape and we draw a systematic phase diagram of the instability. A simple theoretical model allows us to derive a relation between the elongation of the droplet and the amplitude of the Faraday wave, in good agreement with measurements of both quantities.

cond-mat.soft↗

arXiv2016

Reduction in Tension and Stiffening of Lipid Membranes in an Electric Field Revealed by X-ray Scattering

The effect of AC electric fields on the elasticity of supported lipid bilayers has been investigated at the microscopic level using grazing incidence synchrotron x-ray scattering. A strong decrease in the membrane tension up to 1mN/m and a dramatic increase of its effective rigidity up to 300kBT are observed for local electric potentials seen by the membrane < 1V. The experimental results were analyzed using detailed electrokinetic modeling and non-linear Poisson-Boltzmann theory. Based on a modeling of the electromagnetic stress which provides an accurate description of bilayer separation vs pressure curves, we show that the decrease in tension results from the amplification of charge fluctuations on the membrane surface whereas the increase in bending rigidity results from direct interaction between charges in the electric double layer. These effects eventually lead to a destabilization of the bilayer and vesicle formation. Similar effects are expected at the tens of nanometer lengthscale in cell membranes with lower tension, and could explain a number of electrically driven processes.

cond-mat.soft↗

arXiv2013

Controlling interactions in supported bilayers from weak electrostatic repulsion to high osmotic pressure

Understanding interactions between membranes requires measurements on well-controlled systems close to natural conditions, in which fluctuations play an important role. We have determined, by grazing incidence X-ray scattering, the interaction potential between two lipid bilayers, one adsorbed on a solid surface and the other floating close by. We find that interactions in this highly hydrated model system are two orders of magnitude softer than in previously reported work on multilayer stacks. This is attributed to the weak electrostatic repulsion due to the small fraction of ionized lipids in supported bilayers with a lower number of defects. Our data are consistent with the Poisson-Boltzmann theory, in the regime where repulsion is dominated by the entropy of counter ions. We also have unique access to very weak entropic repulsion potentials, which allowed us to discriminate between the various models proposed in the literature. We further demonstrate that the interaction potential between supported bilayers can be tuned at will by applying osmotic pressure, providing a way to manipulate these model membranes, thus considerably enlarging the range of biological or physical problems that can be addressed.

cond-mat.soft↗

arXiv2009

Supported bilayers: combined specular and diffuse x-ray scattering

A new method is proposed for the analysis of specular and off-specular reflectivity from supported lipid bilayers. Both thermal fluctuations and the "static" roughness induced by the substrate are carefully taken into account. Examples from supported bilayers and more complex systems comprising a bilayer adsorbed or grafted on the substrate and another "floating" bilayer are given. The combined analysis of specular and off-specular reflectivity allows the precise determination of the structure of adsorbed and floating bilayers, their tension, bending rigidity and interaction potentials. We show that this new method gives a unique opportunity to investigate phenomena like protusion modes of adsorbed bilayers and opens the way to the investigation of more complex systems including different kinds of lipids, cholesterol or peptides.

cond-mat.soft↗

arXiv2006

Effect of an electric field on a floating lipid bilayer: a neutron reflectivity study

We present here a neutron reflectivity study of the influence of an alternative electric field on a supported phospholipid double bilayer. We report for the first time a reproducible increase of the fluctuation amplitude leading to the complete unbinding of the floating bilayer. Results are in good agreement with a semi-quantitative interpretation in terms of negative electrostatic surface tension.

cond-mat.soft↗

arXiv2003

Swelling of phospholipid floating bilayers: the effect of chain length

The equilibrium distance between two lipid bilayers stable in bulk water and in proximity of a substrate was investigated. Samples consisted of a homogeneous lipid bilayer, floating near an identical bilayer deposited on the hydrophilic surface of a silicon single crystal. Lipids were saturated di-acyl phosphocholines, with the number of carbon atoms per chain, n, varying from 16 to 20. The average and r.m.s. positions of the floating bilayer were determined by means of neutron specular reflectivity. Samples were prepared at room temperature (i.e. with the lipids in the gel phase) and measurements performed at various temperatures so that the whole region of transition from gel to fluid phase was explored. Data have been interpreted in terms of competition between the interbilayer potential and membrane fluctuations and used to estimate the bending rigidity of the bilayer.

cond-mat.soft↗