arXiv subjects

Eric Grelet

Publications and source records attributed to Eric Grelet.

At least 19 recordsLinked to original sources

arXiv2026

Light-Activated Self-thermophoretic Janus Nanopropellers

Achieving controlled and directed motion of artificial nanoscale systems in three-dimensional fluid environments remains a key-challenge in active matter, primarily due to the prevailing thermal fluctuations that rapidly randomize the particle trajectories. While significant progress has been made with micrometer-sized particles, imparting sufficient mechanical energy, or self-propulsion, to nanometer-sized particles to overcome Brownian diffusion and enable controlled transport remains a major issue for emerging applications in nanoscience and nanomedicine. Here, we address this challenge by demonstrating the fuel-free, reversible, and tunable active behavior of gold-silica (Au-SiO2) Janus nanoparticles (radius R=33 nm) induced by optical excitation. Using single particle tracking, we provide direct experimental evidence of self-thermophoresis, clearly distinguishing active motion from thermal noise. These light-driven Janus nanoparticles constitute a minimal yet robust photothermal system for investigating active matter and its manipulation at the nanoscale.

cond-mat.soft↗

arXiv2026

From Lyotropic to Thermotropic Behavior: Solvent-Free Liquid Crystalline Phases in Polymer-Surfactant-Conjugated Rod-shaped Colloidal Viruses

Filamentous bacteriophages fd are viral particles, highly monodisperse in size, that have been widely used as a model colloidal system for studying the self-assembly of rod-shaped particles as well as a versatile template in nanoscience. In aqueous suspensions, fd viruses exhibit lyotropic behavior, forming liquid crystalline phases as their concentration increases. Here, we report a solvent-free system displaying thermotropic phase behavior, achieved through covalent coupling of low molecular weight PEG-based polymer surfactant onto the fd virus surface. Upon lyophilization of aqueous suspensions of these polymer-grafted bacteriophages and subsequent thermal annealing, a solvent-free material is obtained, exhibiting both viscoelasticity and, notably, thermotropic liquid crystalline properties. A combination of small-angle X-ray scattering and optical microscopy experiments reveals the formation of an ordered hexagonal mesophase below 30 {\deg}C, which undergoes a melting transition into an isotropic liquid at higher temperatures. Our results demonstrate an efficient approach for converting lyotropic into thermotropic phase behavior in the columnar liquid crystalline phase of filamentous fd colloids. This approach paves the way for extending such functionalization to other technologically relevant rod-like systems, such as carbon nanotubes and cellulose nanocrystals, enabling the introduction of thermotropic properties in anhydrous colloidal materials.

cond-mat.soft↗

arXiv2026

Janus Polymeric Giant Vesicles on Demand: A Predictive Phase Separation Approach for Efficient Formation

Janus particles, with their intrinsic asymmetry, are attracting major interest in various applications, including emulsion stabilization, micro/nanomotors, imaging, and drug delivery. In this context, Janus polymersomes are particularly attractive for synthetic cell development and drug delivery systems. While they can be achieved by inducing a phase separation within their membrane, their fabrication method remains largely empirical. Here, we propose a rational approach, using Flory-Huggins theory, to predict the self-assembly of amphiphilic block copolymers into asymmetric Janus polymersomes. Our predictions are experimentally validated by forming highly stable Janus giant unilamellar vesicles (JGUVs) with a remarkable yield exceeding 90% obtained from electroformation of various biocompatible block copolymers. We also present a general phase diagram correlating mixing energy with polymersome morphology, offering a valuable tool for JGUV design. These polymersomes can be extruded to achieve quasi-monodisperse vesicles while maintaining their Janus-like morphology, paving the way for their asymmetric functionalization and use as active carriers.

cond-mat.soft↗

arXiv2025

Unveiling Crystalline Order from Glassy Behavior of Charged Rods at Very Low Salt Concentrations

Charged colloids can form ordered structures like Wigner crystals or glasses at very low concentrations due to long-range electrostatic repulsions. Here, we combine small-angle x-ray scattering (SAXS) and optical experiments with simulations to investigate the phase behavior of charged rodlike colloids across a wide range of salt concentrations and packing fractions. At ultra low ionic strength and packing fractions, we reveal both experimentally and numerically a direct transition from a nematic to a crystalline smectic-B phase, previously identified as a glass state. This transition, bypassing the smectic-A intermediate phase, results from minimizing Coulomb repulsion and maximizing entropic gains due to fluctuations in the crystalline structure. This demonstrates how long-range electrostatic repulsion significantly alters the phase behavior of rod-shaped particles and highlights its key-role in driving the self-organization of anisotropic particles.

cond-mat.soft↗

arXiv2025

Self-diffusion in isotropic and liquid crystalline phases of fd virus colloidal rods: a combined single particle tracking and differential dynamic microscopy study

In this article, we investigate the dynamics of self-organised suspensions formed by rod-like fd virus colloids. Two methods have been employed for analysing fluorescence microscopy movies: single particle tracking (SPT) in direct space and differential dynamic microscopy (DDM) in reciprocal space. We perform a quantitative analysis on this anisotropic system with complex diffusion across different self-assembled states, ranging from dilute and semi-dilute liquids to nematic and smectic organisations. By leveraging the complementary strengths of SPT and DDM, we provide new insights in the dynamics of viral colloidal rods, such as long time diffusion coefficients in the smectic phase. We further discuss the advantages and limitations of both methods for studying the intricate dynamics of anisotropic colloidal systems.

cond-mat.soft↗

arXiv2024

Elucidating chirality transfer in liquid crystals of viruses

Chirality is ubiquitous in nature across all length scales, with major implications spanning the fields of biology, chemistry and physics to materials science. How chirality propagates from nanoscale building blocks to meso- and macroscopic helical structures remains an open issue. Here, working with a canonical system of filamentous viruses, we demonstrate that their self-assembly into chiral liquid crystal phases quantitatively results from the interplay between two main mechanisms of chirality transfer: electrostatic interactions from the helical charge patterns on the virus surface, and fluctuation-based helical deformations leading to viral backbone helicity. Our experimental and theoretical approach provides a comprehensive framework for deciphering how chirality is hierarchically and quantitatively propagated across spatial scales. Our work highlights the ways in which supramolecular helicity may arise from subtle chiral contributions of opposite handedness which either act cooperatively or competitively, thus accounting for the multiplicity of chiral behaviors observed for nearly identical molecular systems.

cond-mat.soft↗

arXiv2023

M13-phage-based star-shaped particles with internal flexibility

We report on the construction and the dynamics of monodisperse star-shaped particles, mimicking, at the mesoscale, star polymers. Such multi-arm star-like particles result from the self-assembly of gold nanoparticles, forming the core, with tip-linked filamentous viruses - M13 bacteriophages - acting as spines in a sea urchin-like structure. By combining fluorescence and dark-field microscopy with dynamic light scattering, we investigate the diffusion of these hybrid spiny particles. We reveal the internal dynamics of the star particles by probing their central metallic core, which exhibits a hindered motion that can be described as a Brownian particle trapped in a harmonic potential. We therefore show that the filamentous viruses and specifically their tip proteins behave as entropic springs, extending the relevance of the study of such hybrid mesoscopic analogs of star polymers to phage biotechnology.

cond-mat.soft↗

arXiv2023

Synthesis of achiral rod-shaped triazolic molecules and investigation of their striped texture and propeller-patterned nematic droplets

In this study, novel achiral mesogens containing 4,4'-biphenyl central core connected on both sides through an ester function to 1-(4-(alkyloxy)phenyl)-1H-[1,2,3]-triazolyl group have been synthesized and characterized. Different mesophases have been identified, with the appearance of both a periodic striped pattern and propeller-patterned droplets close to the transition between the nematic and the smectic-C phases. This periodic texture has been found to be independent of the geometry of the sample cell. These observations suggest a spontaneous symmetry breaking which can result either from an intrinsic enantioselective self-sorting process with a chirality synchronization mechanism, or from an extrinsic surface mechanism at the interface between the two phases.

cond-mat.soft↗

arXiv2021

When bigger is faster: a self-van Hove analysis of the enhanced self-diffusion of non-commensurate guest particles in smectics

We investigate the anomalous dynamics in smectic phases of short host rods where, counter-intuitively, long guest rod-shaped particles diffusive faster than the short host ones, due to their precise size mismatch. In addition to the previously reported mean-square displacement, we analyze the time evolution of the Self-van Hove functions G(r,t), as this probability density function uncovers intrinsic heterogeneous dynamics. Through this analysis, we show that the dynamics of the host particles parallel to the director becomes non-gaussian and therefore heterogeneous after the nematic-to-smectic-A phase transition, even though it exhibits a nearly diffusive behavior according to its mean-square displacement. In contrast, the non-commensurate guest particles display Gaussian dynamics of the parallel motion, up to the transition to the smectic-B phase. Thus, we show that the Self-van Hove function is a very sensitive probe to account for the instantaneous and heterogeneous dynamics of our system, and should be more widely considered as a quantitative and complementary approach of the classical mean-square displacement characterization in diffusion processes.

cond-mat.soft↗

arXiv2021

Phase behaviour of hard cylinders

Using isobaric Monte Carlo simulations, we map out the entire phase diagram of a system of hard cylindrical particles of length $L$ and diameter $D$, using an improved algorithm to identify the overlap condition between two cylinders. Both the prolate $L/D>1$ and the oblate $L/D<1$ phase diagrams are reported with no solution of continuity. In the prolate $L/D>1$ case, we find intermediate nematic \textrm{N} and smectic \textrm{SmA} phases in addition to a low density isotropic \textrm{I} and a high density crystal \textrm{X} phase, with \textrm{I-N-SmA} and \textrm{I-SmA-X} triple points. An apparent columnar phase \textrm{C} is shown to be metastable as in the case of spherocylinders. In the oblate $L/D<1$ case, we find stable intermediate cubatic \textrm{Cub}, nematic \textrm{N}, and columnar \textrm{C} phases with \textrm{I-N-Cub}, \textrm{N-Cub-C}, and \textrm{I-Cub-C} triple points. Comparison with previous numerical and analytical studies is discussed. The present study, accounting for the explicit cylindrical shape, paves the way to more sophisticated models with important biological applications, such as viruses and nucleosomes.

cond-mat.soft↗

arXiv2020

Depletion-driven Morphological Transitions in Hexagonal Crystallites of Virus Rods

The assembly of nanometer-sized building blocks into complex morphologies is not only of fundamental interest but also plays a key role in material science and nanotechnology. We show that the shape of self-assembled superstructures formed by rod-like viruses can be controlled by tuning the attraction via the depletion interaction between the rods. Using nonadsorbing polymers as a depleting agent, we demonstrate that a hierarchical unidimensional self-organization into crystalline clusters emerges progressively upon increasing depletion attraction -and enhanced growth kinetics. We observe a polymorphic change proceeding from two-dimensional (2D) crystalline monolayers at weak depletion to one-dimensional (1D) columnar fibers at strong depletion, via the formation of smectic fibrils at intermediate depletion strength. A simple theory for reversible polymerization enables us to determine the typical bond energy between monomeric units making up the smectic fibrils. We also demonstrate that gentle flow-assistance can be used to template filament-like structures into highly aligned supported films. Our results showcase a generic bottom-up approach for tuning the morphology of crystalline superstructures through modification of the interaction between non-spherical building blocks. This provides a convenient pathway for controlling self-organization, dimensionality and structure-formation of anisotropic nanoparticles for use in nanotechnology and functional materials.

cond-mat.soft↗

arXiv2020

Speeding up dynamics by tuning the non-commensurate size of rod-like particles in a smectic phase

Using simulations, we study the diffusion of rod-like guest particles in a smectic environment of rod-like host particles. We find that the dynamics of guest rods across smectic layers changes from a fast nematic-like diffusion to a slow hopping-type dynamics via an intermediate switching regime by varying the length of the guest rods with respect to the smectic layer spacing. We determine the optimal rod length that yields the fastest and the slowest diffusion in a lamellar environment. We show that this behavior can be rationalized by a complex 1D effective periodic potential exhibiting two energy barriers, resulting in a varying preferred mean position of the guest particle in the smectic layer. The interplay of these two barriers controls the dynamics of the guest particles yielding a slow, an intermediate and a fast diffusion regime depending on the particle length.

cond-mat.soft↗

arXiv2019

Directing liquid crystalline self-organization of rod-like particles through tunable attractive single tips

Dispersions of rodlike colloidal particles exhibit a plethora of liquid crystalline states, including nematic, smectic A, smectic B, and columnar phases. This phase behavior can be explained by presuming the predominance of hard-core volume exclusion between the particles. We show here how the self-organization of rodlike colloids can be controlled by introducing a weak and highly localized directional attractive interaction between one of the ends of the particles. This has been performed by functionalizing the tips of filamentous viruses by means of regioselectively grafting fluorescent dyes onto them, resulting in a hydrophobic patch whose attraction can be tuned by varying the number of bound dye molecules. We show, in agreement with our computer simulations, that increasing the single tip attraction stabilizes the smectic phase at the expense of the nematic phase, leaving all other liquid crystalline phases invariant. For a sufficiently strong tip attraction, the nematic state may be suppressed completely to get a direct isotropic liquid-to-smectic phase transition. Our findings provide insights into the rational design of building blocks for functional structures formed at low densities.

cond-mat.soft↗

arXiv2019

Rod-Like Virus-Based Multiarm Colloidal Molecules

We report on the construction of multiarm colloidal molecules by tip-linking filamentous bacteriophages, functionalized either by biological engineering or chemical conjugation. The affinity for streptavidin of a genetically modified vector phage displaying Strep-tags fused to one end of the viral particle is measured by determining the dissociation constant, Kd. In order to improve both the colloidal stability and the efficiency of the self-assembly process, a biotinylation protocol having a chemical yield higher than 90% is presented to regioselectively functionalize the cystein residues located at one end of the bacteriophages. For both viral systems, a theoretical comparison is performed by developing a quantitative model of the self-assembly and interaction of the modified viruses with streptavidin compounds, which accurately accounts for our experimental results. Multiarm colloidal structures of different valencies are then produced by conjugation of these tip-functionalized viruses with streptavidin activated nanoparticles. We succeed to form stable virus based colloidal molecules, whose number of arms, called valency, is solely controlled by tuning the molar excess. Thanks to a fluorescent labeling of the viral arms, the dynamics of such systems is also presented in real time by fluorescence microscopy.

cond-mat.soft↗

arXiv2018

Elementary edge and screw dislocations visualized at the lattice periodicity level in smectic phase of colloidal rods

We report on the identification and quantitative characterization of elementary edge and screw dislocations in a colloidal smectic phase of tip-labeled rods. Thanks to the micrometer layer spacing, direct visualization of dislocations has been performed at the \textit{smectic periodicity scale} by optical fluorescence microscopy. As a result, the displacement field around an edge dislocation has been experimentally established and compared with the profile predicted by elastic theory. Elementary screw dislocations have been also evidenced, for which the core size as well as the \textit{in situ} handedness have been determined. Self-diffusion experiments performed at the individual particle level reveal for the first time nematic-like or "melted" ordering of the defect core.

cond-mat.soft↗

arXiv2017

Fast Diffusion of Long Guest Rods in a Lamellar Phase of Short Host Particles

We investigate the dynamic behavior of long guest rod-like particles immersed in liquid crystalline phases formed by shorter host rods, tracking both guest and host particles by fluorescence microscopy. Counter-intuitively, we evidence that long rods diffuse faster than short rods forming the one-dimensional ordered smectic-A phase. This results from the larger and non-commensurate size of the guest particles as compared to the wavelength of the energy landscape set by the lamellar stack of liquid slabs. The long guest particles are also shown to be still mobile in the crystalline smectic-B phase, as they generate their own voids in the adjacent layers.

cond-mat.soft↗

arXiv2015

Electric field induced birefringence in non-aqueous dispersions of mineral nanorods

Lanthanum phosphate (LaPO4) nanorods dispersed in the non-aqueous solvent of ethylene glycol form a system exhibiting large intrinsic birefringence, high colloidal stability and the ability to self-organize into liquid crystalline phases. In order to probe the electro-optical response of these rod dispersions we study here the electric-field-induced birefringence, also called Kerr effect, for a concentrated isotropic liquid state with an in-plane a.c. sinusoidal electric field, in conditions of directly applied (electrodes in contact with the sample) or externally applied (electrodes outside the sample cell) fields. Performing an analysis of the electric polarizability of our rod-like particles in the framework of Maxwell-Wagner-OKonski theory, we account quantitatively for the coupling between the induced steady-state birefringence and the electric field as a function of the voltage frequency for both sample geometries. The switching time of this non-aqueous transparent system has been measured, and combined with its high Kerr coefficients and its features of optically isotropic offstate and athermal phase behavior, this represents a promising proof-of-concept for the integration of anisotropic nanoparticle suspensions into a new generation of electro-optical devices.

cond-mat.soft↗

arXiv2015

Thermotropic Orientational Order of Discotic Liquid Crystals in Nanochannels: An Optical Polarimetry Study and a Landau-de Gennes Analysis

Optical polarimetry measurements of the orientational order of a discotic liquid crystal based on a pyrene derivative and confined in parallel-aligned nanochannels of monolithic mesoporous alumina, silica, and silicon as a function of temperature, channel radius (3 - 22 nm) and surface chemistry reveal a competition of radial and axial columnar order. The evolution of the orientational order parameter of the confined systems is continuous, in contrast to the discontinuous transition in the bulk. For channel radii larger than 10 nm we suggest several, alternative defect structures, which are compatible both with the optical experiments on the collective molecular orientation presented here and with a translational, radial columnar order reported in previous diffraction studies. For smaller channel radii our observations can semi-quantitatively be described by a Landau-de Gennes model with a nematic shell of radially ordered columns (affected by elastic splay deformations) that coexists with an orientationally disordered, isotropic core. For these structures, the cylindrical phase boundaries are predicted to move from the channel walls to the channel centres upon cooling, and vice-versa upon heating, in accord with the pronounced cooling/heating hystereses observed and the scaling behavior of the transition temperatures with channel diameter. The absence of experimental hints of a paranematic state is consistent with a biquadratic coupling of the splay deformations to the order parameter.

cond-mat.soft↗