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Roel P. A. Dullens

Publications and source records attributed to Roel P. A. Dullens.

17 recordsLinked to original sources

Synthetic Quorum Sensing and Absorbing Phase Transitions in Colloidal Active Matter

Unlike biological active matter that constantly adapt to their environment, the motors of synthetic active particles are typically agnostic to their surroundings and merely operate at constant force. Here, we design colloidal active rods capable of modulating their inner activity in response to crowding, thereby enforcing a primitive form of quorum sensing interactions. Through experiments, simulations, and theory we elucidate the impact of these interactions on the phase behavior of isotropic active matter. We demonstrate that, when conditioned to density, motility regulation can either lead to an absorbing phase transition, where all particles freeze their dynamics, or to atypical phase separation, where flat interfaces supporting a net pressure drop are in mechanical equilibrium. Fully active and fully arrested particles can then form heterogeneous patterns ruled by the competition between quorum sensing and mechanical interactions. Beyond the specifics of motile colloids, we expect our findings to apply broadly to adaptive active matter assembled from living or synthetic units.

cond-mat.stat-mech↗

Attraction-enhanced emergence of friction in colloidal matter

How frictional effects emerge at the microscopic level in particulate materials remains a challenging question, particularly in systems subject to thermal fluctuations due to the transient nature of interparticle contacts. Here, we directly relate particle-level frictional arrest to local coordination in an attractive colloidal model system. We reveal that the orientational dynamics of particles slows down exponentially with increasing coordination number due to the emergence of frictional interactions, the strength of which can be tuned simply by varying the attraction strength. Using a simple computer simulation model, we uncover how the interparticle interactions govern the formation of frictional contacts between particles. Our results establish quantitative relations between friction, coordination and interparticle interactions. This is a key step towards using interparticle friction to tune the mechanical properties of particulate materials.

cond-mat.soft↗

Disentangling the Effects of Curvature and Misorientation on the Shrinkage Behavior of Loop-Shaped Grain Boundaries

The material properties of polycrystals are strongly affected by the evolution and coarsening of their internal grain structures. Yet, studying this process is challenging due to the complex interactions within grain boundary networks. Here, we systematically investigate the shrinkage of isolated loop-shaped grain boundaries in 2D colloidal crystals. Unexpectedly, we find that shear coupling decreases with increasing grain misorientation, contrary to geometric predictions. This counterintuitive result is attributed to enhanced concurrent sliding driven by the annihilation of dislocations. Furthermore, by focusing on the evolution of the grain size, we reveal a transition in shrinkage kinetics between small and large loop sizes, offering an explanation for previously observed discrepancies in grain boundary mobility. These findings reveal a more intricate dependence of grain boundary behavior on curvature and misorientation than previously reported, offering new insights into polycrystal coarsening dynamics.

cond-mat.soft↗

Characterization and Optimization of Fluorescent Organosilica Colloids for 3D Confocal Microscopy Prepared Under 'Zero-Flow'

We optimize and characterize the preparation of 3-trimethoxysilyl propylmethacrylate (TPM) colloidal suspensions for three-dimensional confocal microscopy. We revisit a simple synthesis of TPM microspheres by nucleation of droplets from pre-hydrolyzed TPM oil in a 'zero-flow' regime, and demonstrate how precise and reproducible control of particle size may be achieved via single-step nucleation with a focus on how the reagents are mixed. We also revamp the conventional dyeing method for TPM particles to achieve uniform transfer of a fluorophore to the organosilica droplets, improving particle identification. Finally, we illustrate how a ternary mixture of tetralin, trichloroethylene and tetrachloroethylene may be used as a suspension medium which matches the refractive index of these particles while allowing independent control of the density mismatch between particle and solvent.

cond-mat.soft↗

The effect of curvature on the diffusion of colloidal bananas

Anisotropic colloidal particles exhibit complex dynamics which play a crucial role in their functionality, transport and phase behaviour. In this work, we investigate the two-dimensional diffusion of smoothly curved colloidal rods -- also known as colloidal bananas -- as a function of their opening angle, α. We measure the translational and rotational diffusion coefficients of the particles with opening angles ranging from 0° (straight rods) to nearly 360°(closed rings). In particular, we find that the anisotropic diffusion of the particles varies non-monotonically with their opening angle and that the axis of fastest diffusion switches from the long to the short axis of the particles when α>180°. We also find that the rotational diffusion coefficient of nearly closed rings is approximately an order of magnitude higher than that of straight rods of the same length. Finally, we show that the experimental results are consistent with Slender Body Theory, indicating that the dynamical behavior of the particles arises primarily from their local drag anisotropy. These results highlight the impact of curvature on the Brownian Motion of elongated colloidal particles, which must be taken into account when seeking to understand the behaviour of curved colloidal particles.

cond-mat.soft↗

Thermal Regelation of a Single Particle

In this paper we study the process termed thermal regelation at single particle level. We experimentally extract the physical parameters that determine the interactions between ice and the silica particle for the regelation process. As the premelted layer around the particle plays a key role here, we use the extracted parameters to calculate the thickness of this thin premelted layer, at different given particle sizes.

cond-mat.soft↗

Model-free measurement of the pair potential in colloidal fluids using optical microscopy

We report a straightforward, model-free approach for measuring pair potentials from particle-coordinate data, based on enforcing consistency between the pair distribution function measured separately by the distance-histogram and test-particle insertion routes. We demonstrate the method's accuracy and versatility in simulations of simple fluids, before applying it to an experimental system composed of superparamagnetic colloidal particles. The method will enable experimental investigations into many-body interactions and allow for effective coarse-graining of interactions from simulations.

cond-mat.soft↗

Dynamic mode locking in a driven colloidal system: experiments and theory

In this article we examine the dynamics of a colloidal particle driven by a modulated force over a sinusoidal optical potential energy landscape. Coupling between the competing frequencies of the modulated drive and that of particle motion over the periodic landscape leads to synchronisation of particle motion into discrete modes. This synchronisation manifests as steps in the average particle velocity, with mode locked steps covering a range of average driving velocities. The amplitude and frequency dependence of the steps are considered, and compared to results from analytic theory, Langevin Dynamics simulations, and Dynamic Density Functional Theory. Furthermore, the critical driving velocity is studied, and simulation used to extend the range of conditions accessible in experiments alone. Finally, state diagrams from experiment, simulation, and theory are used to show the extent of the dynamically locked modes in two dimensions, as a function of both the amplitude and frequency of the modulated drive.

cond-mat.soft↗

Dynamic heterogeneities and non-Gaussian behavior in two-dimensional randomly confined colloidal fluids

A binary mixture of super-paramagnetic colloidal particles is confined between glass plates such that the large particles become fixed and provide a two-dimensional disordered matrix for the still mobile small particles, which form a fluid. By varying fluid and matrix area fractions and tuning the interactions between the super-paramagnetic particles via an external magnetic field, different regions of the state diagram are explored. The mobile particles exhibit delocalized dynamics at small matrix area fractions and localised motion at high matrix area fractions, and the localization transition is rounded by the soft interactions [T. O. E. Skinner et al, Phys. Rev. Lett. {\bf 111}, 128301 (2013)]. Expanding on previous work, we find the dynamics of the tracers to be strongly heterogeneous and show that molecular dynamics simulations of an ideal gas confined in a fixed matrix exhibit similar behavior. The simulations show how these soft interactions make the dynamics more heterogenous compared to the disordered Lorentz gas and lead to strong non-Gaussian fluctuations.

cond-mat.soft↗

Colloidal particles driven across periodic optical potential energy landscapes

We study the motion of colloidal particles driven by a constant force over a periodic optical potential energy landscape. Firstly, the average particle velocity is found as a function of the driving velocity and the wavelength of the optical potential energy landscape. The relationship between average particle velocity and driving velocity is found to be well described by a theoretical model treating the landscape as sinusoidal, but only at small trap spacings. At larger trap spacings, a non-sinusoidal model for the landscape must be used. Subsequently, the critical velocity required for a particle to move across the landscape is determined as a function of the wavelength of the landscape. Finally, the velocity of a particle driven at a velocity far exceeding the critical driving velocity is examined. Both of these results are again well described by the two theoretical routes, for small and large trap spacings respectively. Brownian motion is found to have a significant effect on the critical driving velocity, but a negligible effect when the driving velocity is high.

cond-mat.soft↗

Thermal analogue of gimbal lock in a colloidal ferromagnetic Janus rod

We report an entropy-driven orientational hopping transition in a magnetically confined colloidal Janus rod. In a magnetic field, the sedimented rod randomly hops between horizontal and vertical states: the latter state comes at a substantial gravitational cost at no reduction of magnetic potential energy. The probability distribution over the angles of the rod shows that the presence of an external magnetic field leads to the emergence of a metastable vertical state separated from the ground state by an effective barrier. This barrier does not come from the potential energy but rather from the vast gain in phase space available to the rod as it approaches the vertical state. The loss of rotational degree of freedom that gives rise to this effect is a statistical mechanical analogue of the phenomenon of gimbal lock from classical mechanics.

cond-mat.soft↗

Self-assembly and crystallisation of indented colloids at a planar wall

We report experimental and simulation studies of the structure of a monolayer of indented ("lock and key") colloids, on a planar surface. On adding a non-absorbing polymer with prescribed radius and volume fraction, depletion interactions are induced between the colloids, with controlled range and strength. For spherical particles, this leads to crystallisation, but the indented colloids crystallise less easily than spheres, in both simulation and experiment. Nevertheless, simulations show that indented colloids do form plastic (rotator) crystals. We discuss the conditions under which this occurs, and the possibilities of lower-symmetry crystal states. We also comment on the kinetic accessibility of these states.

cond-mat.soft↗

A Landau-Squire Nanojet

Fluid jets are found in nature at all length scales, from microscopic to cosmological. Here we report on an electroosmotically driven jet from a single glass nanopore about 75 nm in radius with a maximum flow rate ~15 pL/s. A novel anemometry technique allows us to map out the vorticity and velocity fields that show excellent agreement with the classical Landau-Squire solution of the Navier Stokes equations for a point jet. We observe a phenomenon that we call flow rectification: an asymmetry in the flow rate with respect to voltage reversal. Such a nanojet could potentially find applications in micromanipulation, nanopatterning, and as a diode in microfluidic circuits.

physics.flu-dyn↗

Localization dynamics of fluids in random confinement

The dynamics of two-dimensional fluids confined within a random matrix of obstacles is investigated using both colloidal model experiments and molecular dynamics simulations. By varying fluid and matrix area fractions in the experiment, we find delocalized tracer particle dynamics at small matrix area fractions and localized motion of the tracers at high matrix area fractions. In the delocalized region, the dynamics is subdiffusive at intermediate times, and diffusive at long times, while in the localized regime, trapping in finite pockets of the matrix is observed. These observations are found to agree with the simulation of an ideal gas confined in a weakly correlated matrix. Our results show that Lorentz gas systems with soft interactions are exhibiting a smoothening of the critical dynamics and consequently a rounded delocalization-to-localization transition.

cond-mat.soft↗

Zigzag transitions and nonequilibrium pattern formation in colloidal chains

Paramagnetic colloidal particles that are optically trapped in a linear array can form a zigzag pattern when an external magnetic field induces repulsive interparticle interactions. When the traps are abruptly turned off, the particles form a nonequilibrium expanding pattern with a zigzag symmetry, even when the strength of the magnetic interaction is weaker than that required to break the linear symmetry of the equilibrium state. We show that the transition to the equilibrium zigzag state is always potentially possible for purely harmonic traps. For anharmonic traps that have a finite height, the equilibrium zigzag state becomes unstable above a critical anharmonicity. A normal mode analysis of the equilibrium line configuration demonstrates that increasing the magnetic field leads to a hardening and softening of the spring constants in the longitudinal and transverse directions, respectively. The mode that first becomes unstable is the mode with the zigzag symmetry, which explains the symmetry of nonequilibrium patterns. Our analytically tractable models help to give further insight into the way that the interplay of such factors as the length of the chain, hydrodynamic interactions, thermal fluctuations affect the formation and evolution of the experimentally observed nonequilibrium patterns.

cond-mat.stat-mech↗

Pattern formation in colloidal explosions

We study the non-equilibrium pattern formation that emerges when magnetically repelling colloids, trapped by optical tweezers, are abruptly released, forming colloidal explosions. For multiple colloids in a single trap we observe a pattern of expanding concentric rings. For colloids individually trapped in a line, we observe explosions with a zigzag pattern that persists even when magnetic interactions are much weaker than those that break the linear symmetry in equilibrium. Theory and computer simulations quantitatively describe these phenomena both in and out of equilibrium. An analysis of the mode spectrum allows us to accurately quantify the non-harmonic nature of the optical traps. Colloidal explosions provide a new way to generate well-characterized non-equilibrium behaviour in colloidal systems.

cond-mat.soft↗

Experimental observation of structural crossover in binary mixtures of colloidal hard spheres

Using confocal-microscopy we investigate the structure of binary mixtures of colloidal hard spheres with size ratio q=0.61. As a function of the packing fraction of the two particle species, we observe a marked change of the dominant wavelength in the pair correlation function. This behavior is in excellent agreement with a recently predicted structural crossover in such mixtures. In addition, the repercussions of structural crossover on the real-space structure of a binary fluid are analyzed. We suggest a relation between crossover and the lateral extension of networks containing only equally sized particles that are connected by nearest neighbor bonds. This is supported by Monte-Carlo simulations which are performed at different packing fractions and size ratios.

cond-mat.soft↗