arXiv subjects

Pierre Lidon

Publications and source records attributed to Pierre Lidon.

16 recordsLinked to original sources

arXiv2026

Response of fluorescent molecular rotors in ternary macromolecular mixtures

For a few decades, Fluorescent Molecular Rotors have been commonly employed as local probes of microviscosity in complex materials. However, without proper calibration, relating microviscosity to a physical parameter is unclear, which strongly limits their quantitative use in biological media for instance. In this study, the response of a molecular rotor in binary and ternary macromolecular aqueous solutions of polyethylene glycol (PEG) of different molecular weights is investigated in order to better rationalize the sensitivity of rotors to their cybotactic environment. More precisely, for the investigated composition range of ternary mixtures, it is shown that a linear mixing rule applies for fluorescence lifetime with the proportion of the two PEG, and with an increasing ratio of heavy PEG leading to larger lifetimes. These results allow to test more precisely the free volume theory, which has been proposed in the context of probing glass transition. Analysis show that while this theory semi-quantitatively captures the observation, its precise use raises some questions.

physics.chem-ph↗

arXiv2025

Diffusiophoretic migration of colloidal particles in sucrose gradients

Diffusiophoresis (DP) refers to the migration of particles driven by a solute concentration gradient in a liquid. Observations in the case of molecular neutral solutes are rather scarce, due to the low drift velocities in dilute solutions, and the difficulty in distinguishing DP from other phenomena in concentrated solutions. We investigated experimentally DP of dispersed colloids driven by concentration gradients of sucrose in water at relatively high concentrations, $C \simeq 1$ mol L$^{-1}$. More precisely, we designed a microfluidic chip to impose a time-dependent sucrose gradient in dead-end microchannels with minimized parasitic flows. Significant migration of the particles toward the regions of low sucrose concentration has been observed, with velocities up to a few $\mu$m s$^{-1}$. Particle tracking and Raman confocal spectroscopy were used to measure individual trajectories and the unsteady sucrose concentration profile respectively. The latter is correctly described by a diffusion equation, but with an interdiffusion coefficient that significantly depends on $C$ in the range of concentrations investigated. We then showed that a model of DP based on a steric exclusion of sucrose molecules from the particle surface with an exclusion length $R_i = 5 \pm 0.9$ angstrom (close to the characteristic size of the sucrose molecule), accounts for the observed trajectories. Possible sources for the observed scattering of our experimental data are finally discussed: Brownian motion and advection of the particles by bulk flows driven by diffusioosmosis at the channel walls and buoyancy.

cond-mat.soft↗

arXiv2025

Transient osmotic flows in a microfluidic channel: measurements of solute permeability and reflection coefficients of hydrogel membranes

We first highlight theoretically a microfluidic configuration that allows to measure two fundamental parameters describing mass transport through a membrane: the solute permeability coefficient $\mathcal{L}_D$, and the associated reflection coefficient $\sigma$. This configuration exploits the high confinement of microfluidic geometries to relate these two coefficients to the dynamics of a transient flow induced by forward osmosis through a membrane embedded in a chip. We then applied this methodology to hydrogel membranes photo-crosslinked in a microchannel with \textit{in situ} measurements of osmotically-induced flows. These experiments enable us to estimate $\mathcal{L}_D$ and $\sigma$ and their dependence on the molecular weight of the solute under consideration, ultimately leading to a precise estimate of the molecular weight cut-off of these hydrogel membranes.

cond-mat.soft↗

arXiv2025

Fluorescent molecular rotor-based polymer materials for local microviscosity mapping in microfluidic channels

A viscosity-sensitive monomer consisting of a methacrylate-functionalized julolidone-based molecular rotor (MECVJ) was synthesized and used to obtain viscosity-sensitive polymers (poly(DMA-\textit{s}-MECVJ)). The qualitative properties of the molecular rotor were preserved after its inclusion in the new polymer, in particular the effect of the viscosity of the surrounding medium on the fluorescence lifetime of the rotor. By grafting these polymers onto glass slides, viscosity-sensitive surfaces were obtained, showing good robustness in time after successive use and washing. As proof of concept, these surfaces were used to assemble a microfluidic chip capable of mapping viscosity of fluids flowing inside the channel.

cond-mat.soft↗

arXiv2023

Molecular Rotors for In Situ Viscosity Mapping during Evaporation of Confined Fluid Mixtures

Numerous formulation processes of materials involve a drying step, during which evaporation of a solvent from a multi-component liquid mixture, often confined in a thin film or in a droplet, lead to concentration and assembly of non volatile compounds. While the basic phenomena ruling evaporation dynamics are known, a precise modeling of practical situations is hindered by the lack of tools for local and time-resolved mapping of concentration fields in such confined systems. In this article, the use of Fluorescence Lifetime Imaging Microscopy and of Fluorescent Molecular Rotors is introduced as a versatile, in-situ and quantitative method to map viscosity and concentration fields in confined, evaporating liquids. More precisely, the cases of drying of a suspended liquid film and of a sessile droplet of mixtures of fructose and water is investigated. Measured viscosity and concentration fields allow to characterize drying dynamics, in agreement with simple modeling of the evaporation process.

cond-mat.soft↗

arXiv2022

Molecular rotors for in situ local viscosity mapping in microfluidic chips

In numerous industrial processes involving fluids, viscosity is a determinant factor for reaction rates, flows, drying, mixing, etc. Its importance is even more determinant for phenomena observed are at the micro- and nano- scales as in nanopores or in micro and nanochannels for instance. However, despite notable progresses of the techniques used in microrheology in recent years, the quantification, mapping and study of viscosity at small scales remains challenging. Fluorescent molecular rotors are molecules whose fluorescence properties are sensitive to local viscosity: they thus allow to obtain viscosity maps by using fluorescence microscopes. While they are well-known as contrast agents in bioimaging, their use for quantitative measurements remains scarce. This paper is devoted to the use of such molecules to perform quantitative, \textit{in situ} and local measurements of viscosity in heterogeneous microfluidic flows. The technique is first validated in the well-controlled situation of a microfluidic co-flow, where two streams mix through transverse diffusion. Then, a more complex situation of mixing in passive micromixers is considered and mixing efficiency is characterized and quantified. The methodology developed in this study thus opens a new path for flow characterization in confined, heterogeneous and complex systems.he methodology developed in this study thus opens a new path for flow characterization in confined, heterogeneous micro- and nano- systems.

physics.flu-dyn↗

arXiv2022

Acoustic monitoring of the gelation of a colloidal suspension

Because they are sensitive to mechanical properties of materials and can propagate even in opaque systems, acoustic waves provides us with a powerful characterization tool in numerous fields. Common techniques mostly rely on time-of-flight measurements and do not exploit the spectral content: however, sound speed and attenuation spectra contain rich information. Such an acoustic spectroscopy already exists and allows to retrieve subtle information on systems of well-known physico-chemistry, but modeling becomes out of reach for industrial systems. In this article, we use a simple empirical approach to monitor the gelation of silica suspensions: we show that the gelation time obtained from acoustic measurements is proportional to this determined with more conventional rheological characterization. Such a results thus opens the way for in-situ monitoring of time-evolving systems in industrial context with acoustic methods only.

cond-mat.soft↗

arXiv2021

Non-isothermal effects on water potential measurement in a simple geometry

In this paper, we investigate quantitatively the coupling between gradients of temperature and of chemical or water potential under steady state conditions in the vapor phase. This coupling is important for the measurement and modeling of the dynamics of water in unsaturated environments like soils and plants. We focus on a simple non-equilibrium scenario in which a gradient of temperature exists across an air-filled gap that separates two aqueous phases with no net transfer of water. This scenario is relevant for measurements of the water potential in environmental and industrial contexts. We use a new tool, a microtensiometer, to perform these measurements. We observed variations of water potential with difference of temperature across the air gap of $-\SI{7.9(3)}{\mega\pascal\per\kelvin}$, in agreement with previous measurements. Our result is close to a first order theoretical prediction, highlighting that most of the effect comes from the variation of saturation pressure with temperature. We then show that thermodiffusion (Soret effect) coupled to natural convection could occur in our experiment and discuss how these effects could explain the small discrepancy observed between measurements and first order theoretical prediction.

physics.geo-ph↗

arXiv2020

Mechanics and structure of carbon black gels under high-power ultrasound

Colloidal gels made of carbon black particles dispersed in light mineral oil are "rheo-acoustic" materials, i.e., their mechanical and structural properties can be tuned using high-power ultrasound, sound waves with submicron amplitude and frequency larger than 20~kHz . The effects of high-power ultrasound on the carbon black gel are demonstrated using two experiments: rheology coupled to ultrasound to test for the gel mechanical response and a timeresolved ultra small-angle X-ray scattering experiment (TRUSAXS) coupled to ultrasound to test for structural changes within the gel. We show that high-power ultrasound above a critical amplitude leads to a complex viscoelastic transient response of the gels within a few seconds: a softening of its storage modulus accompanied by a strong overshoot in its loss modulus. Under high-power ultrasound, the gel displays a viscoelastic spectrum with glass-like features and a significant decrease in its yield strain. Those effects are attributed to the formation of intermittent micro-cracks in the bulk of the gel as evidenced by TRUSAXS. Provided that the shear rate is not large enough to fully fluidize the sample, high-power ultrasound also facilitates the flow of the gel, reducing its yield stress as well as increasing the shear-thinning index, thanks again to the formation of micro-cracks.

cond-mat.soft↗

arXiv2020

Rheo-acoustic gels: Tuning mechanical and flow properties of colloidal gels with ultrasonic vibrations

Colloidal gels, where nanoscale particles aggregate into an elastic yet fragile network, are at the heart of materials that combine specific optical, electrical and mechanical properties. Tailoring the viscoelastic features of colloidal gels in real-time thanks to an external stimulus currently appears as a major challenge in the design of "smart" soft materials. Here we introduce "rheo-acoustic" gels, a class of materials that are sensitive to ultrasonic vibrations. By using a combination of rheological and structural characterization, we evidence and quantify a strong softening in three widely different colloidal gels submitted to ultrasonic vibrations (with submicron amplitude and frequency 20-500 kHz). This softening is attributed to micron-sized cracks within the gel network that may or may not fully heal once vibrations are turned off depending on the acoustic intensity. Ultrasonic vibrations are further shown to dramatically decrease the gel yield stress and accelerate shear-induced fluidization. Ultrasound-assisted fluidization dynamics appear to be governed by an effective temperature that depends on the acoustic intensity. Our work opens the way to a full control of elastic and flow properties by ultrasonic vibrations as well as to future theoretical and numerical modeling of such rheo-acoustic gels.

cond-mat.soft↗

arXiv2019

A mesoscale study of creep in a microgel using the acoustic radiation force

We study the motion of a sphere of diameter 330 $μ$m embedded in a Carbopol microgel under the effect of the acoustic radiation pressure exerted by a focused ultrasonic field. The sphere motion within the microgel is tracked using videomicroscopy and compared to conventional creep and recovery measurements performed with a rheometer. We find that under moderate ultrasonic intensities, the sphere creeps as a power law of time with an exponent $α\simeq 0.2$ that is significantly smaller than the one inferred from global creep measurements below the yield stress of the microgel ($α\simeq 0.4$). Moreover, the sphere relaxation motion after creep and the global recovery are respectively consistent with these two different exponents. By allowing a rheological characterization at the scale of the sphere with forces of the order of micronewtons, the present experiments pave the way for acoustic "mesorheology" which probes volumes and forces intermediate between standard macroscopic rheology and classical microrheology. They also open new questions about the effects of the geometry of the deformation field and of the sphere size and surface properties on the creep behaviour of soft materials.

cond-mat.soft↗

arXiv2018

Enhanced oxygen solubility in metastable water under tension

Despite its relevance in numerous natural and industrial processes, the solubility of molecular oxygen has never been directly measured in capillary condensed liquid water. In this article, we measure oxygen solubility in liquid water trapped within nanoporous samples, in metastable equilibrium with a subsaturated vapor. We show that solubility increases two-fold at moderate subsaturations (RH ~ 0.55). This evolution with relative humidity is in good agreement with a simple thermodynamic prediction using properties of bulk water, previously verified experimentally at positive pressure. Our measurement thus verifies the validity of this macroscopic thermodynamic theory to strong confinement and large negative pressures, where ignificant non-idealities are expected. This effect has strong implications for important oxygen-dependent chemistries in natural and technological contexts.

physics.chem-ph↗

arXiv2017

Measurement of the acoustic radiation force on a sphere embedded in a soft solid

The acoustic radiation force exerted on a small sphere located at the focus of an ultrasonic beam is measured in a soft gel. It is proved to evolve quadratically with the local amplitude of the acoustic field. Strong oscillations of the local pressure are observed and attributed to an acoustic Fabry-P{é}rot effect between the ultrasonic emitter and the sphere. Taking this effect into account with a simple model, a quantitative link between the radiation force and the acoustic pressure is proposed and compared to theoretical predictions in the absence of dissipation. The discrepancy between experiment and theory suggests that dissipative effects should be taken into account for fully modeling the observations.

cond-mat.soft↗

arXiv2016

Lecture notes on surface tension

Lecture notes in french of the lecture on surface tension given in 2015 and 2016 at the preparation to "Agrégation de physique" in the Ecole Normale Supérieure de Lyon

cond-mat.soft↗

arXiv2016

Power-law creep and residual stresses in a carbopol microgel

We report on the interplay between creep and residual stresses in a carbopol microgel. When a constant shear stress $σ$ is applied below the yield stress $σ_\text{y}$, the strain is shown to increase as a power law of time, $γ(t)=γ_0 + (t/τ)^α$, with an exponent $α=0.39\pm 0.04$ that is strongly reminiscent of Andrade creep in hard solids. For applied shear stresses lower than some typical value $σ_\text{c}\simeq 0.2 σ_\text{y}$, the microgel experiences a more complex, anomalous creep behaviour, characterized by an initial decrease of the strain, that we attribute to the existence of residual stresses of the order of $σ_\text{c}$ that persist after a rest time under a zero shear rate following preshear. The influence of gel concentration on creep and residual stresses are investigated as well as possible aging effects. We discuss our results in light of previous works on colloidal glasses and other soft glassy systems.

cond-mat.soft↗

arXiv2016

Grains unchained: local fluidization of a granular packing by focused ultrasound

We report experimental results on the dynamics of a granular packing submitted to high-intensity focused ultrasound. Acoustic radiation pressure is shown to remotely induce local rearrangements within a pile as well as global motion around the focal spot in an initially jammed system. We demonstrate that this fluidization process is intermittent for a range of acoustic pressures and hysteretic when the pressure is cycled. Such a first-order-like unjamming transition is reproduced in numerical simulations in which the acoustic pressure field is modeled by a localized external force. Further analysis of the simulated packings suggests that in the intermittent regime unjamming is not associated with any noticeable prior structural signature. A simple two-state model based on effective temperatures is proposed to account for these findings.

cond-mat.soft↗