arXiv subjects

Mathieu Leocmach

Publications and source records attributed to Mathieu Leocmach.

At least 19 recordsLinked to original sources

arXiv2026

Mechanical response of a simple DNA nanostar hydrogel: symptoms of disorder and glassy emergence of solidity

DNA self-assembly is a well-understood nanotechnology to obtain extremely ordered structures from the nanometer to up to the hundred of microns scale. By contrast, DNA hydrogels rely on the disordered assembly of DNA building blocks to reach macroscopic volumes. However, in order to hold the promise of DNA bulk materials, the sequence designer needs a systematic understanding of how macroscopic properties emerge from disorder. Here, we show a method to study systematically the mechanical response of a simple DNA nanostar hydrogel. This method mobilises bulk rheology, dynamic light scattering microrheology, mechanical modeling, as well as thermodynamic calculation and DNA sequence alteration. At low temperatures, we demonstrate a systematic deviation from Maxwell behaviour that is symptomatic of disordered materials. At temperatures much higher than the percolation of the DNA network, we characterise a surprising solid behaviour that we attribute to a glass transition. Our results show the importance of disorder in DNA materials. Furthermore, the method we showcase in this article can be widely applied to more complex DNA materials.

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arXiv2025

Capillary and priming pressures control the penetration of yield-stress fluids through non-wetting 2D meshes

Forcing hydrophilic fluids through hydrophobic porous solids is a recurrent industrial challenge. If the penetrating fluid is Newtonian, the imposed pressure has to overcome the capillary pressure at the fluid-air interface in a pore. The presence of a yield-stress, however, makes the pressure transfer and the penetration significantly more complex. In this study, we experimentally investigate the forced penetration of a water based yield-stress fluid through a regular hydrophobic mesh under quasi-static conditions, combining quantitative pressure measurements and direct visualisation of the penetration process. We reveal that the penetration is controlled by a competition between the yield-stress and two distinct pressures. The capillary pressure, that dictates the threshold at which the yield-stress fluid penetrates the hydrophobic mesh, and a priming pressure, that controls how the fluid advances through it. The latter corresponds to a pressure drop ensuing a local capillary instability, never reported before. Our findings shine a new light on forced imbibition processes, with direct implications on their fundamental understanding and practical engineering.

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arXiv2023

How to steer active colloids up a vertical wall

An important challenge in active matter lies in harnessing useful global work from entities that produce work locally, e.g., via self-propulsion. We investigate here the active matter version of a classical capillary rise effect, by considering a non-phase separated sediment of self-propelled Janus colloids in contact with a vertical wall. We provide experimental evidence of an unexpected and dynamic adsorption layer at the wall. Additionally, we develop a complementary numerical model that recapitulates the experimental observations. We show that an adhesive and aligning wall enhances the pre-existing polarity heterogeneity within the bulk, enabling polar active particles to climb up a wall against gravity, effectively powering a global flux. Such steady-state flux has no equivalent in a passive wetting layer.

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arXiv2022

Aging or DEAD: origin of the non-monotonic response to weak self-propulsion in active glasses

Among amorphous states, glass is defined by relaxation times longer than the observation time. This nonergodic nature makes the understanding of glassy systems an involved topic, with complex aging effects or responses to further out-of-equilibrium external drivings. In this respect active glasses made of self-propelled particles have recently emerged as stimulating systems which broadens and challenges our current understanding of glasses by considering novel internal out-of-equilibrium degrees of freedom. In previous experimental studies we have shown that in the ergodicity broken phase, the dynamics of dense passive particles first slows down as particles are made slightly active, before speeding up at larger activity. Here, we show that this nonmonotonic behavior also emerges in simulations of soft active Brownian particles and explore its cause. We refute that the Deadlock by Emergence of Active Directionality (DEAD) model we proposed earlier describes our data. However, we demonstrate that the nonmonotonic response is due to activity enhanced aging, and thus confirm the link with ergodicity breaking. Beyond self-propelled systems, our results suggest that aging in active glasses is not fully understood.

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arXiv2021

Immersed Cantilever Apparatus for Mechanics and Microscopy

We present here a novel cantilever based apparatus to perform translational stress or strain controlled rheology in very soft solids, and obtain simultaneous confocal imaging of the 3 dimensional microstructure. The stress is measured using eddy based sensors. Both the stress and strain are controlled by applying PID control loops on measured quantities and changing position using a micromanipulator. To get rid of surface tension forces, the sample and cantilever are immersed. This enables stress measurement and control down to 3mPa. With this apparatus, we can independently apply shear and normal stress, or strain, with same precision. We demonstrate the technical capability of the setup with steady shear strain or stress experiments on a soft protein gel system. The simultaneous confocal imaging offers insight into the macroscopic breaking observed in an increasing shear strain experiment.

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arXiv2020

Characterization of the gelation and resulting network of a mixed-protein gel derived from sodium caseinate and ovalbumin in the presence of glucono-$\delta$-lactone

We investigated mixed-protein gels made from sodium caseinate and ovalbumin at different ratios with use of the acidification agent glucono-$\delta$-lactone. Dynamic viscoelastic measurements revealed that increasing the ovalbumin content decreased the mechanical properties of the gel but accelerated onset time of the phase transition. Ultrasound spectroscopy during gelation revealed that the relative velocity gradually decreased, whereas the ultrasonic attenuation increased during the whole acidification process until gelation was complete, although these changes were much smaller than those observed with heat-induced gelation. Confocal laser scanning microscopy along with scanning electron microscopy revealed that although uniform mixing of sodium caseinate and ovalbumin was observed, sodium caseinate is likely to mainly lead formation of the gel network, and the porosity of the resulting gel network depends on the ratio of these two components. The results demonstrate that confocal laser scanning microscopy is a useful tool for analyzing both the networks within mixed-protein gels and the contribution of each protein to the network and gelation.

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arXiv2019

Nonmonotonic behavior in the dense assemblies of active colloids

We study experimentally a sediment of self-propelled Brownian particles with densities ranging from dilute to ergodic supercooled, to nonergodic glass, to nonergodic polycrystal. In a compagnon letter, we observe a nonmonotonic response to activity of relaxation of the nonergodic glass state: a dramatic slowdown when particles become weakly self-propelled, followed by a speedup at higher activities. Here we map ergodic supercooled states to standard passive glassy physics, provided a monotonic shift of the glass packing fraction and the replacement of the ambient temperature by the effective temperature. However we show that this mapping fails beyond glass transition. This failure is responsible for the nonmonotonic response. Furthermore, we generalize our finding by examining the dynamical response of an other class of nonergodic systems : polycrystals. We observe the same nonmonotinic response to activity. To explain this phenomenon, we measure the size of domains were particles move in the same direction. This size also shows a nonmonotonic response, with small lengths corresponding to slow relaxation. This suggests that the failure of the mapping of nonergodic active states to a passive situation is general and is linked to anisotropic relaxation mechanisms specific to active matter.

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arXiv2019

Active glass: ergodicity breaking dramatically affects response to self-propulsion

We study experimentally the response of a dense sediment of Brownian particles to self-propulsion. We observe that the ergodic supercooled liquid relaxation is monotonically enhanced by activity. By contrast the nonergodic glass shows an order of magnitude slowdown at low activities with respect to passive case, followed by fluidization at higher activities. Our results contrast with theoretical predictions of the ergodic approach to glass transition summing up to a shift of the glass line. We propose that nonmonotonicity is due to competing effects of activity: (i) extra energy that helps breaking cages (ii) directionality that hinders cage exploration. We call it "Deadlock from the Emergence of Active Directionality" (DEAD). It suggests further theoretical works should include thermal motion.

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arXiv2019

Irreversible hardening of a colloidal gel under shear: the smart response of natural rubber latex gels

Natural rubber is obtained by processing natural rubber latex, a liquid colloidal suspension that rapidly gels after exudation from the tree. We prepared such gels by acidification, in a large range of particle volume fractions, and investigated their rheological properties. We show that natural rubber latex gels exhibit a unique behavior of irreversible strain hardening: when subjected to a large enough strain, the elastic modulus increases irreversibly. Hardening proceeds over a large range of deformations in such a way that the material maintains an elastic modulus close to, or slightly higher than the imposed shear stress. Local displacements inside the gel are investigated by ultrasound imaging coupled to oscillatory rheometry, together with a Fourier decomposition of the oscillatory response of the material during hardening. Our observations suggest that hardening is associated with irreversible local rearrangements of the fractal structure, which occur homogeneously throughout the sample.

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arXiv2018

Gelation as condensation frustrated by hydrodynamics and mechanical isostaticity

Colloidal gels have unique mechanical and transport properties that stem from their bicontinous nature, in which a colloidal network is intertwined with a viscous solvent, and have found numerous applications in foods, cosmetics, construction materials, and for medical applications, such as cartilage replacements. So far, our understanding of the process of colloidal gelation is limited to long-time dynamical effects, where gelation is viewed as a phase separation process interrupted by the glass transition. However, this picture neglects two important effects: the influence of hydrodynamic interactions, and the emergence of mechanical stability. With confocal microscopy experiments, here we successfully follow the entire process of gelation with a single-particle resolution, yielding time-resolved measures of internal stress and viscoelasticity from the very beginning of the aggregation process. First, we demonstrate that the incompressible nature of a liquid component constrains the initial stage of phase separation, assisting the formation of a percolated network. Then we show that this network is not mechanically stable and undergoes rearrangements driven by self-generated internal stress. Finally, we show that mechanical metastability is reached only after percolation of locally isostatic environments, proving isostaticity a necessary condition for the stability and load bearing ability of gels rather than the glass transition. Our work reveals the crucial roles of momentum conservation in gelation in addition to the conventional purely out-of-equilibrium thermodynamic picture.

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arXiv2018

Formation of porous crystals via viscoelastic phase separation

Viscoelastic phase separation of colloidal suspensions can be interrupted to form gels either by glass transition or by crystallization. With a new confocal microscopy protocol, we follow the entire kinetics of phase separation, from homogeneous phase to different arrested states. For the first time in experiments, our results unveil a novel crystallization pathway to sponge-like porous crystal structures. In the early stages, we show that nucleation requires a structural reorganization of the liquid phase, called stress-driven ageing. Once nucleation starts, we observe that crystallization follows three different routes: direct crystallization of the liquid phase, Bergeron process, and Ostwald ripening. Nucleation starts inside the reorganised network, but crystals grow past it by direct condensation of the gas phase on their surface, driving liquid evaporation, and producing a network structure different from the original phase separation pattern. We argue that similar crystal-gel states can be formed in monoatomic and molecular systems if the liquid phase is slow enough to induce viscoelastic phase separation, but fast enough to prevent immediate vitrification. This provides a novel pathway to form nano-porous crystals of metals and semiconductors without dealloying, which may be important for catalytic, optical, sensing, and filtration applications.

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arXiv2016

Ion pairing controls rheological properties of "processionary" polyelectrolyte hydrogels

We demonstrated recently that polyelectrolytes with cationic moieties along the chain and a single anionic head are able to form physical hydrogels due to the reversible nature of the head-to-body ionic bond. Here we generate a variety of such polyelectrolytes with various cationic moieties and counterion combinations starting from a common polymeric platform. We show that the rheological properties (shear modulus, critical strain) of the final hydrogels can be modulated over three orders of magnitude depending on the cation/anion pair. Our data fit remarkably well within a scaling model involving a supramolecular head-to-tail single file between cross-links, akin to the behaviour of pine-processionary caterpillar. This model allows the quantitative measure of the amount of counterion condensation from standard rheology procedure.

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arXiv2015

Local Oscillatory Rheology from Echography

Local Oscillatory Rheology from Echography (LORE) consists in a traditional rheology experiment synchronized with high-frequency ultrasonic imaging which gives access to the local material response to oscillatory shear. Besides classical global rheological quantities, this method provides quantitative time-resolved information on the local displacement across the entire gap of the rheometer. From the local displacement response, we compute and decompose the local strain in its Fourier components and measure the spatially-resolved viscoelastic moduli. After benchmarking our method on homogeneous Newtonian fluids and soft solids, we demonstrate that this technique is well suited to characterize spatially heterogeneous samples, wall slip, and the emergence of nonlinearity under large amplitude oscillatory stress in soft materials.

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arXiv2015

Differential Dynamic Microscopy to characterize Brownian motion and bacteria motility

We have developed a lab work module where we teach undergraduate students how to quantify the dynamics of a suspension of microscopic particles, measuring and analyzing the motion of those particles at the individual level or as a group. Differential Dynamic Microscopy (DDM) is a relatively recent technique that precisely does that and constitutes an alternative method to more classical techniques such as dynamics light scattering (DLS) or video particle tracking (VPT). DDM consists in imaging a particle dispersion with a standard light microscope and a camera. The image analysis requires the students to code and relies on digital Fourier transform to obtain the intermediate scattering function, an autocorrelation function that characterizes the dynamics of the dispersion. We first illustrate DDM on the textbook case of colloids where we measure the diffusion coefficient. Then we show that DDM is a pertinent tool to characterize biologic systems such as motile bacteria i.e.bacteria that can self propel, where we not only determine the diffusion coefficient but also the velocity and the fraction of motile bacteria. Finally, so that our paper can be used as a tutorial to the DDM technique, we have joined to this article movies of the colloidal and bacterial suspensions and the DDM algorithm in both Matlab and Python to analyze the movies.

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arXiv2015

High-throughput and long-term observation of compartmentalized biochemical oscillators

We report the splitting of an oscillating DNA circuit into $\sim 700$ droplets with picoliter volumes. Upon incubation at constant temperature, the droplets display sustained oscillations that can be observed for more than a day. Superimposed to the bulk behaviour, we find two intriguing new phenomena - slow desynchronization between the compartments and kinematic spatial waves - and investigate their possible origin. This approach provides a route to study the influence of small volume effects in biology, and paves the way to technological applications of compartmentalized molecular programs controlling complex dynamics.

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arXiv2014

Mediating gel formation from structurally controlled poly(electrolytes) through multiple "head-to-body" electrostatic interactions

Tuning the chain-end functionality of a short-chain cationic homopolymer, owing to the nature of the initiator used in the ATRP polymerisation step, can be used to mediate the formation of a gel of this poly(electrolyte) in water. While a neutral end group gives a solution of low viscosity, a highly homogeneous gel is obtained with a phosphonate anionic moiety, as characterized by rheometry and diffusion NMR. This novel type of supramolecular control over poly(electrolytic) gel formation could find potential use in a variety of applications in the field of electroactive materials.

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arXiv2014

Creep and Fracture of a Protein Gel under Stress

Biomaterials such as protein or polysaccharide gels are known to behave qualitatively as soft solids and to rupture under an external load. Combining optical and ultrasonic imaging to shear rheology we show that the failure scenario of a protein gel is reminiscent of brittle solids: after a primary creep regime characterized by a power-law behavior which exponent is fully accounted for by linear viscoelasticity, fractures nucleate and grow logarithmically perpendicularly to shear, up to the sudden rupture of the gel. A single equation accounting for those two successive processes nicely captures the full rheological response. The failure time follows a decreasing power law with the applied shear stress, similar to the Basquin law of fatigue for solids. These results are in excellent agreement with recent fiber-bundle models that include damage accumulation on elastic fibers and exemplify protein gels as model, brittle-like soft solids.

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arXiv2014

Novel zone formation due to interplay between sedimentation and phase ordering

Usually, we expect large particles to sediment faster than small of the same material. Contrary to this intuition, we report a dynamical competition between sedimentation and phase ordering which leads to smaller particles settling faster than larger ones. We access this phenomenon using suspensions of polymers and two colloidal species which we image with confocal microscopy. Polymers mediate attractions between colloids, leading to phase separation and crystallisation. We find that the dynamical interplay between sedimentation, phase separation and crystal nucleation underlie this phenomenon. Furthermore, under certain conditions we find a kinetic pathway leading to an apparent coexistence between a one component crystal and binary fluid of equal buoyancy. These findings may be relevant to the basic understanding of sedimentation-induced zone formation in nature and industrial applications.

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