The relaxation dynamics of a model fluid of platelike colloidal particles is investigated by means of a phenomenological dynamic density functional theory. The model fluid approximates the particles within the Zwanzig model of restricted orientations. The driving force for time-dependence is expressed completely by gradients of the local chemical potential which in turn is derived from a density functional -- hydrodynamic interactions are not taken into account. These approximations are expected to lead to qualitatively reliable results for low densities as those within the isotropic-nematic two-phase region. The formalism is applied to model an initially spatially homogeneous stable or metastable isotropic fluid which is perturbed by switching a two-dimensional array of Gaussian laser beams. Switching on the laser beams leads to an accumulation of colloidal particles in the beam centers. If the initial chemical potential and the laser power are large enough a preferred orientation of particles occurs breaking the symmetry of the laser potential. After switching off the laser beams again the system can follow different relaxation paths: It either relaxes back to the homogeneous isotropic state or it forms an approximately elliptical high-density core which is elongated perpendicular to the dominating orientation in order to minimize the surface free energy. For large supersaturations of the initial isotropic fluid the high-density cores of neighboring laser beams of the two-dimensional array merge into complex superstructures.
Nonequilibrium steady states in an open system connecting two reservoirs of platelike colloidal particles are investigated by means of a recently proposed phenomenological dynamic density functional theory [M. Bier and R. van Roij, Phys. Rev. E 76, 021405 (2007)]. The platelike colloidal particles are approximated within the Zwanzig model of restricted orientations, which exhibits an isotropic-nematic bulk phase transition. Inhomogeneities of the local chemical potential generate a diffusion current which relaxes to a nonvanishing value if the two reservoirs coupled to the system sustain diffe…
Structural relaxation in hard-sphere colloidal glasses has been studied using confocal microscopy. The motion of individual particles is followed over long time scales to detect the rearranging regions in the system. We have used normal mode analysis to understand the origin of the rearranging regions. The low frequency modes, obtained over short time scales, show strong spatial correlation with the rearrangements that happen on long time scales.
Understanding relaxation of supercooled fluids is a major challenge and confining such systems can lead to bewildering behaviour. Here we exploit an optically confined colloidal model system in which we use reduced pressure as a control parameter. The dynamics of the system are ``Arrhenius'' at low and moderate pressure, but at higher pressures relaxation is faster than expected. We associate this faster relaxation with a decrease in density adjacent to the confining boundary due to local ordering in the system enabled by the flexible wall.
We investigate the stress relaxation behavior on the application of step strains to aging aqueous suspensions of the synthetic clay Laponite. The stress exhibits a two-step decay, from which the slow relaxation modes are extracted as functions of the sample ages and applied step strain deformations. Interestingly, the slow time scales that we estimate show a dramatic enhancement with increasing strain amplitudes. We argue that the system ends up exploring the deeper sections of its energy landscape following the application of the step strain.
A universal secondary relaxation process, known as the Johari-Goldstein (JG) $β$-relaxation process, appears in glass formers. It involves all parts of the molecule and is particularly important in glassy systems because of its very close relationship with the $α$-relaxation process. However, the absence of a J-G $β$-relaxation mode in colloidal glasses raises questions regarding its universality. In the present work, we study the microscopic relaxation processes in Laponite suspensions, a model soft glassy material, by dynamic light scattering (DLS) experiments. $α$ and $β$-relaxation timesca…
The rheology of dense amorphous materials under large shear strain is not fully understood, partly due to the difficulty of directly viewing the microscopic details of such materials. We use a colloidal suspension to simulate amorphous materials, and study the shear-induced structural relaxation with fast confocal microscopy. We quantify the plastic rearrangements of the particles in several ways. Each of these measures of plasticity reveals spatially heterogeneous dynamics, with localized regions where many particles are strongly rearranging by these measures. We examine the shapes of these r…
Using high-speed confocal microscopy, we measure the particle positions in a colloidal suspension under large amplitude oscillatory shear. Using the particle positions we quantify the in situ anisotropy of the pair-correlation function -- a measure of the Brownian stress. From these data, we find two distinct types of responses as the system crosses over from equilibrium to far-from-equilibrium states. The first is a nonlinear amplitude saturation that arises from shear-induced advection, while the second is a linear frequency saturation due to competition between suspension relaxation and she…
In polymers melts and supercooled liquids, the glassy dynamics is characterized by the rattling of monomers or particles in the cage formed by their neighbors. Recently, a direct correlation in such systems, described by a universal scaling form, has been established between the rattling amplitude and the structural relaxation time. In this paper we analyze the glassy dynamics emerging from the formation of a persistent network in a model colloidal gel at very low density. The structural relaxation time of the gel network is compared with the mean squared displacement at short times, correspon…
Spherical colloidal crystals (CCs) self-assemble on the interface between two liquids. These 2D structures unconventionally combine local hexagonal order and spherical geometry. Nowadays CCs are actively studied by altering their structures. However, the statistical analysis of such experiments results is limited by uniqueness of self-assembled structures and their short lifetime. Here we perform numerical experiments to investigate pathways of CC structure relaxation after the intrusion of interstitial. The process is simulated in the frames of overdamped molecular dynamics method. The relaxa…
Understanding the relaxation dynamics of colloidal suspensions is crucial to identify the elements that influence the mobility of their constituents, assess their macroscopic response across the relevant time and length scales, and thus disclose the fundamentals underpinning their exploitation in formulation engineering. In this work, we specifically assess the impact of long-ranged ordering on the relaxation dynamics of suspensions of soft-repulsive rod-like particles, which are able to self-organise into nematic and smectic liquid-crystalline phases. By performing Dynamic Monte Carlo simulat…
Vapour deposition can directly produce ultrastable glasses, which are similar to conventional glasses aged over thousands of years. The highly mobile surface layer is believed to accelerate the ageing process of vapour-deposited glasses, but its microscopic kinetics has not been experimentally observed. Here we studied the deposition growth kinetics of a two-dimensional colloidal glass at the single-particle level using video microscopy. We found that newly deposited particles in the surface layer (depth $d<14$ particles) relaxed via frequent out-of-cage motions, while particles in the deeper …
Although glassy relaxation is typically associated with disorder, here we report on a new type of glassy dynamics relating to dislocations within 2-D crystals of colloidal dimers. Previous studies have demonstrated that dislocation motion in dimer crystals is restricted by certain particle orientations. Here, we drag an optically trapped particle through such dimer crystals, creating dislocations. We find a two-stage relaxation response where initially dislocations glide until encountering particles that cage their motion. Subsequent relaxation occurs logarithmically slowly through a second pr…
We present thermophoretic measurements in aqueous suspensions of three different polystyrene (PS) particles of varying negative charge, size and surface coating. Our measurement technique is based on the observation of the colloidal steady-state distribution using conventional bright-field microscopy, which avoids undesirable effects such as laser-induced convection or local heating. We find that the colloids with the weakest zeta potential exhibit the strongest thermophoretic effect, suggesting that surface functionality leads to a more intricate dependence of the Soret coefficient on hydrody…
We experimentally study the transient motion of a colloidal particle actively dragged by an optical trap through different viscoelastic fluids (wormlike micelles, polymer solutions, and entangled $λ$-phage DNA). We observe that, after sudden removal of the moving trap, the particle recoils due to the recovery of the deformed fluid microstructure. We find that the transient dynamics of the particle proceeds via a double exponential relaxation, whose relaxation times remain independent of the initial particle velocity whereas their amplitudes strongly depend on it. While the fastest relaxation m…
The time-dependent structure, interfacial tension, and evaporation of an oversaturated colloid-rich (liquid) phase in contact with an undersaturated colloid-poor (vapor) phase of a colloidal dispersion is investigated theoretically during the early-stage relaxation, where the interface is relaxing towards a local equilibrium state while the bulk phases are still out of equilibrium. Since systems of this type exhibit a clear separation of colloidal and solvent relaxation time scales with typical times of interfacial tension measurements in between, they can be expected to be suitable for analog…
The aging dynamics of colloidal suspensions of Laponite, a synthetic clay, is investigated using dynamic light stattering (DLS) and viscometry after a quench into the glassy phase. DLS allows to follow the diffusion of Laponite particles and reveals that there are two modes of relaxation. The fast mode corresponds to a rapid diffusion of particles within "cages" formed by the neighboring particles. The slow mode corresponds to escape from the cages: its average relaxation time increases exponentially fast with the age of the glass. In addition, the slow mode has a broad distribution of relaxat…
Phase equilibria between regions of different thickness in thin liquid films stabilized by colloidal particles are investigated using a quasi-two-dimensional thermodynamic formalism. Appropriate equilibrium conditions for the film tension, normal pressure, and chemical potential of the particles in the film are formulated, and it is shown that the relaxation of these parameters occurs consecutively on three distinct time scales. Film stratification is described quantitatively for a hard-sphere suspension using a Monte-Carlo method to evaluate thermodynamic equations of state. Coexisting phases…
Recent theories predict that when a supercooled liquid approaches the glass transition, particle clusters with a special "amorphous order" nucleate within the liquid, which lead to static correlations dictating the dramatic slowdown of liquid relaxation. The prediction, however, has yet to be verified in 3D experiments. Here, we design a colloidal system, where particles are confined inside spherical cavities with an amorphous layer of particles pinned at the boundary. Using this novel system, we capture the amorphous-order particle clusters and demonstrate the development of a static correlat…
We study the relaxation of a single colloidal sphere which is periodically driven between two nonequilibrium steady states. Experimentally, this is achieved by driving the particle along a toroidal trap imposed by scanned optical tweezers. We find that the relaxation time after which the probability distributions have been relaxed is identical to that obtained by a steady state measurement. In quantitative agreement with theoretical calculations the relaxation time strongly increases when driving the system further away from thermal equilibrium.
We examine the structure and dynamics of small isolated $N$-particle clusters interacting via short-ranged Morse potentials. "Ideally preprared ensembles" obtained via exact enumeration studies of sticky hard sphere packings serve as reference states allowing us to identify key statistical-geometrical properties and to quantitatively characterize how nonequilibrium ensembles prepared by thermal quenches at different rates $\dot{T}$ differ from their equilibrium counterparts. Studies of equilibrium dynamics show nontrival temperature dependence: nonexponential relaxation indicates both glassy d…
We theoretically study the effect of external deformation on activated structural relaxation and elementary aspects of the nonlinear mechanical response of glassy hard sphere fluids in the context of the nonequilibrium version of the Elastically Collective Nonlinear Langevin Equation (ECNLE) theory. ECNLE theory describes activated relaxation as a coupled local-nonlocal event involving local caging and longer range collective elasticity, with the latter becoming more important with increasing packing fraction. The central new question is how this physical picture, and the relative importance o…
The adsorption dynamics of a colloidal particle at a fluid interface is studied theoretically and numerically, documenting distinctly different relaxation regimes. The adsorption of a perfectly smooth particle is characterized by a fast exponential relaxation to thermodynamic equilibrium where the interfacial free energy has a minimum. The short relaxation time is given by the ratio of viscous damping to capillary forces. Physical and/or chemical heterogeneities in a colloidal system, however, can result in multiple minima of the free energy giving rise to metastability. In the presence of met…
We present here a microscopic study of the effect of shear on a dense purely repulsive colloidal suspension. We use Multispeckle Diffusing Wave Spectroscopy to monitor the transient motions of colloidal particles after being submitted to an oscillatory strain. This technique proves efficient to record the time evolution of the relaxation times distribution. After a high oscillatory shear, we show that this distribution displays a full aging behavior. Oppositely, when a moderate shear is applied the distribution is modified in a non trivial way. Whereas high shear is able to erase all the sampl…
Dilute Laponite suspensions in water at low salt concentration form repulsive colloidal glasses which display physical aging. This phenomenon is still not completely understood and in particular, little is known about the connection between the flow history, as a determinant of the initial state of the system, and the subsequent aging dynamics. Using a stress controlled rheometer, we perform stress jump experiments to observe the elastic component of the flow stress that remains on cessation of flow or flow quenching. We investigate the connection between the dynamics of these residual stresse…
The primary and secondary relaxation timescales of aging colloidal suspensions of Laponite are estimated from intensity autocorrelation functions obtained in dynamic light scattering (DLS) experiments. The dynamical slowing down of these relaxation processes are compared with observations in fragile supercooled liquids by establishing a one-to-one mapping between the waiting time since filtration of a Laponite suspension and the inverse of the temperature of a supercooled liquid that is rapidly quenched towards its glass transition temperature. New timescales, such as the Vogel time and the Ka…
We use molecular dynamics computer simulations to investigate the relaxation dynamics of a simple model for a colloidal gel at a low volume fraction. We find that due to the presence of the open spanning network this dynamics shows at low temperature a non-trivial dependence on the wave-vector which is very different from the one observed in dense glass-forming liquids. At high wave vectors the relaxation is due to the fast cooperative motion of the branches of the gel network, whereas at low wave vectors the overall rearrangements of the heterogeneous structure produce the relaxation process.
Colloidal gel aging is investigated using very long runs of brownian dynamics simulations. The Asakura Oosawa description of the depletion interaction is used to model a simple colloid polymer mixture. Several regimes are identified during gel formation. The Intermediate scattering function displays a double decay characteristic of systems where some kinetic processes are frozen. The $β$ relaxation at short times is explained in terms of the Krall-Weitz model for the decorelation due to the elastic modes present. The $α$ relaxation at long times is well described by a stretched exponential, sh…
The slow dynamics for a colloidal suspension of particles interacting with a hard-core repulsion complemented by a short-ranged attraction is discussed within the frame of mode-coupling theory for ideal glass transitions for parameter points near a higher-order glass-transition singularity. The solutions of the equations of motion for the density correlation functions are solved for the square-well system in quantitative detail by asymptotic expansion using the distance of the three control parameters packing fraction, attraction strength and attraction range from their critical values as smal…
We report the modifications of the microscopic dynamics of a colloidal glass submitted to shear. We use multispeckle diffusing wave spectroscopy to monitor the evolution of the spontaneous slow relaxation processes after the sample have been submitted to various straining. We show that high shear rejuvenates the system and accelerates its dynamics whereas moderate shear overage the system. We analyze this phenomena within the frame of the Bouchaud's trap model.
We investigate the gel formation from the equilibrium sol phase in a simple model that has the characteristics of (colloidal) gel-forming systems at a finite temperature. At low volume fraction and low temperatures, particles are linked by long-living bonds and form an open percolating network. By means of molecular dynamics simulations, we study the lifetime of bonds and nodes of the gel network in order to relate these quantities to the complex relaxation dynamics observed.
The reversible aggregates formation in a shear thickening, concentrated colloidal suspension is investigated through speckle visibility spectroscopy, a dynamic light scattering technique recently introduced [P.K. Dixon and D.J. Durian, Phys. Rev. Lett. 90, 184302 (2003)]. Formation of particles aggregates is observed in the jamming regime, and their relaxation after shear cessation is monitored as a function of the applied shear stress. The aggregates relaxation time increases when a larger stress is applied. Several phenomena have been proposed to interpret this behavior: an increase of the a…
We study the formation of bands of colloidal particles driven by periodic external fields. Using Brownian dynamics, we determine the dependence of the band width on the strength of the particle interactions and on the intensity and periodicity of the field. We also investigate the switching (field-on) dynamics and the relaxation times as a function of the system parameters. The observed scaling relations were analyzed using a simple dynamic density-functional theory of fluids.
Microscopic relaxation timescales are estimated from the autocorrelation functions obtained by dynamic light scattering experiments for Laponite suspensions with different concentrations ($C_{L}$), added salt concentrations ($C_{S}$) and temperatures ($T$). It has been shown in an earlier work [Soft Matter, 10, 3292-3300 (2014)] that the evolutions of relaxation timescales of colloidal glasses can be compared with molecular glass formers by mapping the waiting time ($t_{w}$) of the former with the inverse of thermodynamic temperature ($1/T$) of the latter. In this work, the fragility parameter…
Silica nanoparticles trapped at air-water interface form a 2D solid state with amorphous order. We propose a theoretical model to describe how this solid-like state deforms under a shear strain ramp up to and beyond a yielding point which leads to plastic flow. The model accounts for all the particle-level and many-body physics of the system: nonaffine displacements, local connectivity and its evolution in terms of cage-breaking, and interparticle interactions mediated by the particle chemistry and colloidal forces. The model is able to reproduce experimental data with only two non-trivial fit…
Results of the idealized mode-coupling theory for the structural relaxation in suspensions of hard-sphere colloidal particles are presented and discussed with regard to recent light scattering experiments. The structural relaxation becomes non-diffusive for long times, contrary to the expectation based on the de Gennes narrowing concept. A semi-quantitative connection of the wave vector dependences of the relaxation times and amplitudes of the final $α$-relaxation explains the approximate scaling observed by Segr{è} and Pusey [Phys. Rev. Lett. {\bf 77}, 771 (1996)]. Asymptotic expansions lead …
The adsorption of single colloidal microparticles (0.5--1 $μ$m radius) at a water-oil interface has been recently studied experimentally using digital holographic microscopy [Kaz \textit{et al., Nat. Mater.}, 2012, \textbf{11}, 138--142]. An initially fast adsorption dynamics driven by capillary forces is followed by an unexpectedly slow relaxation to equilibrium that is logarithmic in time and can span hours or days. The slow relaxation kinetics has been attributed to the presence of surface "defects" with nanoscale dimensions (1--5\,nm) that induce multiple metastable configurations of the c…
We extend the classical Gouy-Chapman model of two planar parallel interacting double-layers, which is used as a first approximation to describe the force between colloidal particles, by considering the finite-thickness of the colloids. The formation of two additional double layers due to this finite thickness, modifies the interaction force compared to the Gouy-Chapman case, in which the colloids are semi-infinite objects. In this paper we calculate this interaction force and some other size-dependent properties using a mean field level of description, based on the Poisson-Boltzmann (PB) equat…
Colloidal particles are considered ideal building blocks to produce materials with enhanced physical properties. The state-of-the-art techniques for synthesizing these particles provide control over shape, size, and directionality of the interactions. In spite of these advances, there is still a huge gap between the synthesis of individual components and the management of their spontaneous organization towards the desired structures. The main challenge is the control over the dynamics of self-organization. In their kinetic route towards thermodynamically stable structures, colloidal particles …
We present experimental confirmation of dynamic facilitation in monodisperse and bidisperse colloidal suspensions near the glass transition volume fraction. Correlations in particle dynamics are seen to exist not only in space (clusters and strings) but also as bubbles in space-time. Quantitatively, highly mobile particles are more likely (than immobile particles) to have nearest neighbors that were highly mobile in immediately preceding times. The interpretation is that a particle's mobility enables or facilitates the subsequent motion of its neighbors. Facilitation is most pronounced at the …
One of the greatest challenges in contemporary condensed matter physics is to ascertain whether the formation of glasses from liquids is fundamentally thermodynamic or dynamic in origin. While the thermodynamic paradigm has dominated theoretical research for decades, the purely kinetic perspective of the dynamical facilitation (DF) theory has attained prominence in recent times. In particular, recent experiments and simulations have highlighted the importance of facilitation using simple model systems composed of spherical particles. However, an overwhelming majority of liquids possess anisotr…
Dynamic Light Scattering (DLS) measurements were performed on colloidal suspensions of Laponite\textsuperscript{\textregistered} at different concentrations in the range $C_\text{w}= (1.5÷3.0)$%. The slowing down of the dynamics induced by aging was monitored by following the temporal evolution of autocorrelation functions at different concentrations towards the gel and glass transition. Exploiting analogies with supercooled liquids approaching their glass transitions, an Angell plot for the structural relaxation times was drawn. Finally, the fragility of Laponite\textsuperscript{\textregister…
A scaling model is developed to correlate relaxation time distribution of soft glassy materials to ultimate recovery. We propose that in the limit of creep-recovery time smaller than age, time translational invariance can be applied to ageing soft materials. In such limit, multimode linear viscoelastic model with Spriggs relaxation spectrum predicts enhancement in the ultimate recovery with broadening of the relaxation time distribution. We analyze these results in the context of creep-recovery behavior of aqueous suspension of laponite with varying concentration of salt.
Previous experiments have shown that spherical colloidal particles relax to equilibrium slowly after they adsorb to a liquid-liquid interface, despite the large interfacial energy gradient driving the adsorption. The slow relaxation has been explained in terms of transient pinning and depinning of the contact line on the surface of the particles. However, the nature of the pinning sites has not been investigated in detail. We use digital holographic microscopy to track a variety of colloidal spheres---inorganic and organic, charge-stabilized and sterically stabilized, aqueous and non-aqueous--…
Crystalline bilayers of charged colloidal suspensions which are confined between two parallel plates and sheared via a relative motion of the two plates are studied by extensive Brownian dynamics computer simulations. The charge-stabilized suspension is modeled by a Yukawa pair potential. The unsheared equilibrium configuration are two crystalline layers with a nested quadratic in-plane structure. For increasing shear rates $\dot γ$, we find the following steady states: first, there is a static solid which is elastically sheared until a yield-stress limit is reached. Then there are two crystal…
Stress relaxation in crystalline solids is mediated by the formation and diffusion of defects. While it is well established how externally-generated stresses relax, through the proliferation and motion of dislocations in the lattice, it remains relatively unknown how crystals cope with internal stresses. We investigate, both experimentally and in simulations, how highly localized stresses relax in two-dimensional soft colloidal crystals. When a single particle is actively excited, by means of optical tweezing, a rich variety of highly collective stress relaxation mechanisms results. These mani…
A Rayleigh-Taylor-like instability of a dense colloidal layer under gravity in a capillary of microfluidic dimensions is considered. We access all relevant lengthscales with particle-level microscopy and computer simulations which incorporate long-range hydrodynamic interactions between the particles. By tuning the gravitational driving force, we reveal a mechanism whose growth is connected to the fluctuations of specific wavelengths, non-linear pattern formation and subsequent diffusion-dominated relaxation. Our linear stability theory captures the initial regime and thus predicts mixing cond…
Microgel particles composed of Interpenetrated Polymer Networks (IPN) of poly(N-isopropylacrylamide) (PNIPAM) and poly(acrylic acid) (PAAc) dispersed in water have been investigated through dynamic light scattering. The study of the temperature, concentration and pH dependence of the relaxation time has highlighted the existence of a thermoreversible transition corresponding to the swollen-shrunken volume phase transition. The presence of PAAc introduces an additional pH-sensitivity with respect to the temperature-sensitivity due to PNIPAM and leads to interesting differences in the transition…
We monitor the relaxation of internal stresses in a fractal colloidal gel on cessation of flow and find a weak power law decay, $σ_i \sim t^{-α}$ over 5 decades of time where $α\approx 0.07$. The system exhibits physical aging of the elastic modulus, $G' \sim t^β$, with $β\approx α$. Imposition of zero stress after waiting time $t_w$ results in strain recovery as the system relaxes without constraint. Remarkably, recoveries at different $t_w$ can be shifted to construct a master curve where data are scaled vertically by $1/σ_i(t_w)$ and plotted horizontally as $(t-t_w)/t_w^μ$ where $μ\approx 1…
The yet virtually unexplored class of soft colloidal rods with small aspect ratio is investigated and shown to exhibit a very rich phase and dynamic behavior, spanning from liquid to nearly melt state. Instead of nematic order, these short and soft nanocylinders alter their organization with increasing concentration from isotropic liquid with random orientation to one with preferred local orientation and eventually a multi-domain arrangement with local orientational order. The latter gives rise to a kinetically suppressed state akin to structural glass with detectable terminal relaxation, whic…
An aqueous suspension of the synthetic clay Laponite undergoes a transition from a liquid-like ergodic state to a glass-like nonergodic arrested state. In an observation that closely resembles the dynamical slowdown observed in supercooled liquids, the phenomenon of kinetic arrest in Laponite suspensions is accompanied by a growth in the $α$-relaxation time with increasing sample aging time, $t_{w}$. The ubiquitous dynamic slowdown and fragile behavior observed in glass forming liquids approaching the glass transition is typically ascribed to the growth in the size of distinct dynamical hetero…
We provide a detailed derivation of a recently developed first-principles approach to calculating averages in systems of interacting, spherical Brownian particles under time-dependent flow. Although we restrict ourselves to flows which are both homogeneous and incompressible, the time-dependence and geometry (e.g. shear, extension) are arbitrary. The approximations formulated within mode-coupling theory are particularly suited to dense colloidal suspensions and capture the slow relaxation arising from particle interactions and the resulting glass transition to an amorphous solid. The delicate …
We propose a microscopic picture for understanding the nonlinear rheology of supercooled liquids with soft-repulsive potentials. Based on Brownian dynamics simulations of supercooled charge-stabilized colloidal suspensions, our analysis shows that the shear thinning of viscosity (eta) at large enough shear rates (sr), expressed as eta~sr^(-lambda), originates from the evolution of the localized elastic region (LER). An LER is a transient region composed of the first several coordination shells of a reference particle. In response to the external shear, particles within LER undergo nearly affin…
We perform Dynamic Monte Carlo simulations to investigate the equilibrium dynamics of hard colloidal cuboids in oblate and prolate nematic liquid crystals. In particular, we characterise the particles' diffusion along the nematic director and perpendicularly to it, and observe a structural relaxation decay that strongly depend on the particle anisotropy. To assess the Gaussianity of their dynamics and eventual occurrence of collective motion, we calculate two- and four-point correlation functions that incorporate the instantaneous values of the diffusion coefficients parallel and perpendicular…
Transport properties of a hard-sphere colloidal fluid are investigated by Brownian dynamics simulations. We implement a novel algorithm for the time-dependent velocity-autocorrelation function (VACF) essentially eliminating the noise of the bare random motion. The measured VACF reveals persistent anti-correlations manifested by a negative algebraic power-law tail $t^{-5/2}$ at all densities. At small packing fractions, the simulations fully agree with the analytic low-density prediction, yet the amplitude of the tail becomes dramatically suppressed as the packing fraction is increased. The mod…
To gain insight into the kinetics of colloidal gel evolution at low particle volume fractions $ϕ$, we utilize differential dynamic microscopy to investigate particle aggregation, geometric percolation, and the subsequent transition to nonergodic dynamics. We report the emergence of unexpectedly rich multiscale dynamics upon the onset of nonergodicity, which separates the wave vectors $q$ into three different regimes. In the high-$q$ domain, the gel exhibits $ϕ$-independent internal vibrations of fractal clusters. The intermediate-$q$ domain is dominated by density fluctuations at the length sc…
Yielding is central to the relaxation, flow and fracture of a wide range of soft and molecular glasses, but its microscopic origin remains unclear. Here, we elucidate the yielding of a colloidal glass by using x-ray scattering to monitor the structure factor during the yielding process. We apply a recently introduced combination of small-angle x-ray scattering and rheology to the oscillatory shear, and follow the structure factor during the increasing strain amplitude. Surprisingly, we observe a sharp transition in the orientational ordering of the nearest-neighbor structure upon yielding, in …
In event-chain Monte Carlo simulations we model colloidal particles in two dimensions that interact according to an isotropic short-ranged pair potential which supports the two typical length scales present in decagonal quasicrystals. We investigate the assembled structures as we vary the density and temperature. Our special interest is related to the transition from quasicrystal to liquid. We find a one-step first-order melting transition without a pentahedratic phase as predicted within the KTHNY melting theory for quasicrystals. However, we discover that the slow relaxation of phasonic flip…
