arXiv subjects

Jan Vermant

Publications and source records attributed to Jan Vermant.

12 recordsLinked to original sources

arXiv2026

Thermo-Rheological Memory of $\kappa$-Carrageenan Fluid Gels Formed Under Flow

Fluid gels are soft materials formed by shearing biopolymer solutions during the sol-gel transition. Their ability to yield and flow beyond a critical stress makes them attractive for designing versatile, biocompatible materials in food, health care and medical applications. Although it is well established that both microstructure and mechanical properties depend on the shear applied during gelation, a unified physical framework linking these features remains lacking. Here, using $\kappa$-carrageenan gels as a model system, we use a combination of rheology and confocal microscopy to tackle their shear-induced structuring in fluid gels. We identify a thermo-rheological memory in $\kappa$-carrageenan gels formed under flow and show that it arises from a competition between shear and interparticle adhesion, captured by an Adhesion number. The resulting microstructural evolution is reminiscent of the behavior of attractive particulate dispersions under simple shear flow, thereby bridging gels made of macromolecules and particulate gels. This framework provides a route to tune fluid gel properties without altering their composition.

cond-mat.soft↗

arXiv2026

Orthogonal Superposition Rheometry of soft core-shell microgels

The mechanisms of flow in suspensions of soft particles above the glass-transition volume fraction and in the jammed state were probed using Orthogonal Superposition Rheometry (OSR). A small amplitude oscillatory shear flow is superimposed orthogonally onto a steady shear flow, which allows monitoring the viscoelastic spectra of sheared jammed core-shell microgels during flow. The characteristic crossover frequency {\omega}c, deduced from the viscoelastic spectrum, provides information about the shear induced structural relaxation time, which is connected to the microscopic yielding mechanism of cage breaking. The shear rate evolution of the crossover frequency is used to achieve a superposition of all spectra and get a better insight of the flow mechanism. Despite their inherent softness, the hybrid core-shell microgels exhibit similarities with hard sphere-like flow behavior, with the main difference that for the microgels the transition from a glassy to a jammed state introduces a volume fraction dependence of the scaling of {\omega}c with shear rate. We further check the application of the Kramers-Kronig relations on the experimental low strain amplitude OSR data finding a good agreement. Finally, the low frequency response at high strain rates was investigated with open bottom cell geometry and instrumental limits were identified. Based on these limits, we discuss previous OSR data and findings in repulsive and attractive colloidal glasses, and compared them with the current soft particle gels.

cond-mat.soft↗

arXiv2024

Unifying atoms and colloids near the glass transition through bond-order topology

In this combined experimental and simulation study, we utilize bond-order topology to quantitatively match particle volume fraction in mechanically uniformly compressed colloidal suspensions with temperature in atomistic simulations. The obtained mapping temperature is above the dynamical glass transition temperature, indicating that the colloidal systems examined are structurally most like simulated undercooled liquids. Furthermore, the structural mapping procedure offers a unifying framework for quantifying relaxation in arrested colloidal systems.

cond-mat.soft↗

arXiv2024

Comparative Analysis of Fluctuations in Viscoelastic Stress: A Comparison of the Temporary Network and Dumbbell models

Traditionally, stress fluctuations in flowing and deformed materials are overlooked, with an obvious focus on average stresses in a continuum mechanical approximation. However, these fluctuations, often dismissed as noise, hold the potential to provide direct insights into the material structure and its structure-stress coupling, uncovering detailed aspects of fluid transport and relaxation behaviors. Despite advancements in experimental techniques allowing for the visualization of these fluctuations, their significance remains largely untapped, as modeling efforts continue to target Newtonian fluids within the confines of Gaussian noise assumptions. In the present work a comparative analysis of stress fluctuations in two distinct microstructural models is carried out: the temporary network model and the dumbbell model. Despite both models conforming to the Upper Convected Maxwell Model at a macroscopic level, the temporary network model predicts non-Gaussian fluctuations. We find that stress fluctuations within the temporary network model exhibit more pronounced abruptness at local scale, with only an enlargement of the control volume leading to a gradual Gaussian-like noise, diminishing the differences between the two models. These findings underscore the heightened sensitivity of fluctuating rheology to microstructural details and the microstructure-flow coupling, beyond what is captured by macroscopically averaged stresses.

cond-mat.mtrl-sci↗

arXiv2023

Ductile-to-brittle transition and yielding in soft amorphous materials: perspectives and open questions

Soft amorphous materials are viscoelastic solids ubiquitously found around us, from clays and cementitious pastes to emulsions and physical gels encountered in food or biomedical engineering. Under an external deformation, these materials undergo a noteworthy transition from a solid to a liquid state that reshapes the material microstructure. This yielding transition was the main theme of a workshop held from January 9 to 13, 2023 at the Lorentz Center in Leiden. The manuscript presented here offers a critical perspective on the subject, synthesizing insights from the various brainstorming sessions and informal discussions that unfolded during this week of vibrant exchange of ideas. The result of these exchanges takes the form of a series of open questions that represent outstanding experimental, numerical, and theoretical challenges to be tackled in the near future.

cond-mat.soft↗

arXiv2023

Surface-Sensitive Raman Scattering by Transferable Nanoporous Plasmonic Membranes

Raman spectroscopy is a powerful technique to characterize materials. It probes non-destructively chemical composition, crystallinity, defects, strain and coupling phenomena. However, the Raman response of surfaces or thin films is often weak and obscured by dominant bulk signals. Here we overcome this limitation by placing a transferable porous gold membrane (PAuM) on top of the surface of interest. Slot-like nanopores in the membrane act as plasmonic slot antennas and enhance the Raman response of the surface or thin film underneath. Simultaneously, the PAuM suppresses the penetration of the excitation laser into the bulk, efficiently blocking the bulk Raman signal. Using graphene as a model surface, we show that these two simultaneous effects lead to an increase in the surface-to-bulk Raman signal ratio by three orders of magnitude. We find that 90% of the Raman enhancement occurs within the top 2.5 of the material, demonstrating truly surface-sensitive Raman scattering. To validate our approach, we analyze the surface of a LaNiO3 thin film. We observe a Raman mode splitting for the LaNiO3 surface-layer, which is spectroscopic evidence that the surface structure differs from the bulk. This result underpins that PAuM give direct access to Raman signatures of surfaces and their structural properties.

cond-mat.mtrl-sci↗

arXiv2020

Light-switchable propulsion of active particles with reversible interactions

Active systems such as microorganisms and self-propelled particles show a plethora of collective phenomena, including swarming, clustering, and phase separation. Control over the propulsion direction and switchability of the interactions between the individual self-propelled units may open new avenues in designing of materials from within. Here, we present a self-propelled particle system, consisting of half-gold coated titania ($\mathrm{TiO}_2$) particles, in which we can fast and on-demand reverse the propulsion direction, by exploiting the different photocatalytic activities on both sides. We demonstrate that the reversal in propulsion direction changes the nature of the hydrodynamic interaction from attractive to repulsive and can drive the particle assemblies to undergo both fusion and fission transitions. Moreover, we show these active colloids can act as nucleation sites, and switch rapidly the interactions between active and passive particles, leading to reconfigurable assembly and disassembly. Our experiments are qualitatively described by a minimal hydrodynamic model.

cond-mat.soft↗

arXiv2019

Sculpting vesicles with active particles: Less is more

Biological cells are able to generate intricate structures and respond to external stimuli, sculpting their membrane from within. Simplified biomimetic systems can aid in understanding the principles which govern these shape changes and elucidate the response of the cell membrane under strong deformations. Here, a combined experimental and simulation approach is used to identify the conditions under which different non-equilibrium shapes and distinct active shape fluctuations can be obtained by enclosing self-propelled particles in giant vesicles. Interestingly, the most pronounced shape changes are observed at relatively low particle loadings, starting with the formation of tether-like protrusions to highly branched, dendritic structures. At high volume fractions, globally deformed vesicle shapes are observed. The obtained state diagram of vesicles sculpted by active particles predicts the conditions under which local internal forces can generate dramatic cell shape changes, such as branched structures in neurons.

cond-mat.soft↗

arXiv2018

Effects of particle stiffness on the extensional rheology of model rod-like nanoparticle suspensions

The linear and nonlinear rheological behavior of two rod-like particle suspensions as a function of concentration is studied using small amplitude oscillatory shear, steady shear and capillary breakup extensional rheometry. The rod-like suspensions are composed of fd virus and its mutant fdY21M, which are perfectly monodisperse, with a length on the order of 900 nm. The particles are semi flexible yet differ in their persistence length. The effect of stiffness on the rheological behavior in both, shear and extensional flow, is investigated experimentally. The linear viscoelastic shear data is compared in detail with theoretical predictions for worm-like chains. The extensional properties are compared to Batchelor's theory, generalized for the shear thinning nature of the suspensions. Theoretical predictions agree well with the measured complex moduli at low concentrations as well as the nonlinear shear and elongational viscosities at high flow rates. The results in this work provide guidelines for enhancing the elongational viscosity based on purely frictional effects in absence of strong normal forces which are characteristic for high molecular weight polymers.

cond-mat.soft↗

arXiv2014

Surfactant-induced rigidity of interfaces: a unified approach to free and dip-coated films

The behavior of thin liquid films is known to be strongly affected by the presence of surfactants at the interfaces. The detailed mechanism by which the latter enhance film stability is still a matter of debate, in particular concerning the influence of surface elastic effects on the hydrodynamic boundary condition at the liquid/air interfaces. In the present work, "twin" hydrodynamic models neglecting surfactant transport to the interfaces are proposed to describe the coating of films onto a solid plate (Landau-Levich-Derjaguin configuration) as well as soap film pulling (Frankel configuration). Experimental data on the entrained film thickness in both configurations can be fitted very well using a single value of the surface elasticity, which is in good agreement with independent measurements by mean of surface expansion experiments in a Langmuir through. The analysis shows how and when the soap films or dip coating experiments may be used to precisely and sensitively measure the surface elasticity of surfactant solutions.

cond-mat.soft↗

arXiv2010

A model for colloidal suspension under magnetohydrodynamic conditions

We present a comprehensive model to account for the behavior of suspended nanoparticles under magnetohydrodynamic conditions. The Lorentz force not only drags nanoparticle flocs toward the walls reducing the distance between flocs resulting a more negative total pair interaction potential energy, but also produces extra magnetic-induced stresses inside a floc leading to a change of pair interaction distance thus giving rise to a less negative total potential energy. The model explains quite well the recent experimental results showing that magnetic field assists aggregation in laminar or weak turbulent flows, but favors floc disruption in turbulent regime.

cond-mat.soft↗

arXiv2005

Flow behavior of colloidal rod-like viruses in the nematic phase

The behavior of a colloidal suspension of rod-like {\it fd} viruses in the nematic phase, subjected to steady state and transient shear flows is studied. The monodisperse nature of these rods combined with relatively small textural contribution to the overall stress make this a suitable model system to investigate the effects of flow on the non-equilibrium phase diagram. Transient rheological experiments are used to determine the critical shear rates at which director tumbling, wagging and flow-aligning occurs. The present model system enables us to study the effect of rod concentration on these transitions. The results are in quantitatively agreement with the Doi-Edwards-Hess model. Moreover, we observe that there is a strong connection between the dynamic transitions and structure formation, which is not incorporated in theory.

cond-mat.soft↗