arXiv subjects

C. Patrick Royall

Publications and source records attributed to C. Patrick Royall.

At least 37 records · Page 2Linked to original sources

arXiv2022

The glass transition in molecules, colloids and grains: universality and specificity

We highlight certain key achievements in experimental work on molecular, colloidal and granular glassformers. This short review considers these three classes of experimental systems and focusses largely on the work of the authors and their coworkers and thus is far from exhaustive. Our goal is rather to discuss particular experimental results from these classes and to explore universality and specificity across the broad range of length- and time-scales they span. We emphasize that a variety of phenomena, not least dynamical heterogeneity, growing lengthscales and a change in structure, albeit subtle, are now well established in these three classes of glassformer. We then review some experimental measurements which depend more specifically on the class of glassformer, such as the Gardner transition and some which have been investigated more in one or two classes than in all, such as configurational entropy and evidence for a dynamical phase transition. We finally put forward some open questions and consider what could be done to fill some of the gaps between theoretical approaches and experiments.

cond-mat.soft↗

arXiv2022

Many-body correlations are non-negligible in both fragile and strong glassformers

It is widely believed that the emergence of slow glassy dynamics is encoded in a material's microstructure. First-principles theory [mode-coupling theory (MCT)] is able to predict the dramatic slowdown of the dynamics from only static two-point correlations as input, yet it cannot capture all of the observed dynamical behavior. Here we go beyond two-point spatial correlation functions by extending MCT systematically to include higher-order static and dynamic correlations. We demonstrate that only adding the static triplet direct correlations already qualitatively changes the predicted glass-transition diagram of binary hard spheres and silica. Moreover, we find a non-trivial competition between static triplet correlations that work to stabilize the glass state, and dynamic higher-order correlations which destabilize it for both materials. We conclude that the conventionally neglected static triplet direct correlations as well as higher-order dynamic correlations are in fact non-negligible in both fragile and strong glassformers.

cond-mat.soft↗

arXiv2022

The rheology of confined colloidal hard discs

Colloids may be treated as `big atoms' so that they are good models for atomic and molecular systems. Colloidal hard disks are therefore good models for 2d materials and although their phase behavior is well characterized, rheology has received relatively little attention. Here we exploit a novel, particle-resolved, experimental set-up and complementary computer simulations to measure the shear rheology of quasi-hard-disc colloids in extreme confinement. In particular, we confine quasi-2d hard discs in a circular `corral' comprised of 27 particles held in optical traps. Confinement and shear suppress hexagonal ordering that would occur in the bulk and create a layered fluid. We measure the rheology of our system by balancing drag and driving forces on each layer. Given the extreme confinement, it is remarkable that our system exhibits rheological behavior very similar to unconfined 2d and 3d hard particle systems, characterized by a dynamic yield stress and shear-thinning of comparable magnitude. By quantifying particle motion perpendicular to shear, we show that particles become more tightly confined to their layers with no concomitant increase in density upon increasing shear rate. Shear thinning is therefore a consequence of a reduction in dissipation due to a weakening in interactions between layers as the shear rate increases. We reproduce our experiments with Brownian Dynamics simulations with Hydrodynamic Interactions (HI) included at the level of the Rotne-Prager tensor. That the inclusion of HI is necessary to reproduce our experiments is evidence of their importance in transmission of momentum through the system.

cond-mat.soft↗

arXiv2022

Steering self-organisation through confinement

Self-organisation is the spontaneous emergence of spatio-temporal structures and patterns from the interaction of smaller individual units. Examples are found across many scales in very different systems and scientific disciplines, from physics, materials science and robotics to biology, geophysics and astronomy. Recent research has highlighted how self-organisation can be both mediated and controlled by confinement. Confinement occurs through interactions with boundaries, and can function as either a catalyst or inhibitor of self-organisation. It can then become a means to actively steer the emergence or suppression of collective phenomena in space and time. Here, to provide a common framework for future research, we examine the role of confinement in self-organisation and identify overarching scientific challenges across disciplines that need to be addressed to harness its full scientific and technological potential. This framework will not only accelerate the generation of a common deeper understanding of self-organisation but also trigger the development of innovative strategies to steer it through confinement, with impact, e.g., on the design of smarter materials, tissue engineering for biomedicine and crowd management.

nlin.AO↗

arXiv2022

Direct Imaging of Contacts and Forces in Colloidal Gels

Colloidal dispersions are prized as model systems to understand basic properties of materials, and are central to a wide range of industries from cosmetics to foods to agrichemicals. Among the key developments in using colloids to address challenges in condensed matter is to resolve the particle coordinates in 3D, allowing a level of analysis usually only possible in computer simulation. However in amorphous materials, relating mechanical properties to microscopic structure remains problematic. This makes it rather hard to understand, for example, mechanical failure. Here we address this challenge by studying the contacts and the forces between particles, as well as their positions. To do so, we use a colloidal model system (an emulsion) in which the interparticle forces and local stress can be linked to the microscopic structure. We demonstrate the potential of our method to reveal insights into the failure mechanisms of soft amorphous solids by determining local stress in a colloidal gel. In particular, we identify `force chains' of load-bearing droplets, and local stress anisotropy, and investigate their connection with locally rigid packings of the droplets.

cond-mat.soft↗

arXiv2022

Modelling the filtration efficiency of a woven fabric: The role of multiple lengthscales

During the COVID-19 pandemic, many millions have worn masks made of woven fabric, to reduce the risk of transmission of COVID-19. Masks are essentially air filters worn on the face, that should filter out as many of the dangerous particles as possible. Here the dangerous particles are the droplets containing virus that are exhaled by an infected person. Woven fabric is unlike the material used in standard air filters. Woven fabric consists of fibres twisted together into yarns that are then woven into fabric. There are therefore two lengthscales: the diameters of: (i) the fibre and (ii) the yarn. Standard air filters have only (i). To understand how woven fabrics filter, we have used confocal microscopy to take three dimensional images of woven fabric. We then used the image to perform Lattice Boltzmann simulations of the air flow through fabric. With this flow field we calculated the filtration efficiency for particles a micrometre and larger in diameter. In agreement with experimental measurements by others, we find that for particles in this size range, filtration efficiency is low. For particles with a diameter of 1.5 micrometres our estimated efficiency is in the range 2.5 to 10%. The low efficiency is due to most of the air flow being channelled through relatively large (tens of micrometres across) inter-yarn pores. So we conclude that fabric is expected to filter poorly due to the hierarchical structure of woven fabrics.

physics.flu-dyn↗

arXiv2022

How effective are face coverings in reducing transmission of COVID-19?

In the COVID-19 pandemic, billions are wearing face masks, in both health care settings and in public. Which type of mask we should wear in what situation, is therefore important. There are three basic types: cotton, surgical, and respirators (e.g. FFP2, N95 and similar). All are essentially air filters worn on the face. Air filtration is relatively well understood, however, we have almost no direct evidence on the relative role played by aerosol particles of differing sizes in disease transmission. But if the virus concentration is assumed independent of aerosol particle size, then most virus will be in particles > 1 $μ$m. We develop a model that predicts surgical masks are effective at reducing the risk of airborne transmission because the filtering material most surgical masks use is highly effective at filtering particles with diameters > 1 $μ$m. However, surgical masks are significantly less effective than masks of FFP2, N95 and similar standards, mostly due to the poor fit of surgical masks. Earlier work found that ~30% of the air bypasses a surgical mask and is not filtered. This highlights the fact that standards for surgical masks do not specify how well the mask should fit, and so are not adequate for protection against COVID-19.

cond-mat.soft↗

arXiv2021

Towards the ideal glass transition by pinning in a dimer-polymer mixture

We use a mixture of a polymer and its dimer to control dynamics in a manner inspired by \emph{pinning} a fraction of the system. In our system of $α$-methyl styrene, where the polymer has a glass transition at higher temperature than the dimer, at intermediate temperatures, the polymer acts to "pin" the dimer. Within this temperature range, we use differential scanning calorimetry to infer a point-to-set length which we find to be profoundly influenced by the degree of pinning. We determine the dynamics of the system with dielectric spectroscopy and find that while the dynamics are very substantially slowed by the "pinning", the fragility exhibits only a small change relative to the precision of our measurements. This may indicate that in the approach we have used, fragility has a relatively weak dependence on quantities such as the point--to--set length. % than one might expect, However, an alternative explanation is that the dimer may act to \emph{plasticize} the polymer and thus open routes to relaxation that may be inaccessible to fully pinned systems.

cond-mat.soft↗

arXiv2021

Crystal polymorph selection mechanism of hard spheres hidden in the fluid

Nucleation plays a critical role in the birth of crystals and is associated with a vast array of phenomena such as protein crystallization and ice formation in clouds. Despite numerous experimental and theoretical studies, many aspects of the nucleation process like the polymorph selection mechanism in the early stages are far from being understood. Here, we show that the excess of particles in a face-centred-cubic (fcc)-like environment with respect to those in a hexagonal-close-packed (hcp)-like environment in a crystal nucleus of hard spheres as observed in simulations and experiments can be explained by the higher order structure in the fluid phase. We show using both simulations and experiments that, in the metastable fluid phase, fivefold symmetry clusters -- pentagonal bipyramids (PBs) -- known to be inhibitors of crystal nucleation, transform into a different cluster -- Siamese dodecahedra (SDs). Due to their geometry, these clusters form a bridge between the fivefold symmetric fluid and the fcc crystal, thus lowering its interfacial free energy with respect to the hcp crystal, and shedding new light on the polymorph selection mechanism.

cond-mat.soft↗

arXiv2021

Crystallisation and Polymorph Selection in Active Brownian Particles

We explore crystallisation and polymorph selection in active Brownian particles with numerical simulation. In agreement with previous work [Wysocki $\textit{et al.}$ $\textit{Europhys. Lett.}$, $\textbf{105}$ 48004 (2014)], we find that crystallisation is suppressed by activity and occurs at higher densities with increasing $Péclet$ number ($Pe$). While the nucleation rate decreases with increasing activity, the crystal growth rate increases due to the accelerated dynamics in the melt. As a result of this competition we observe the transition from a nucleation and growth regime at high $Pe$ to "spinodal nucleation" at low $Pe$. Unlike the case of passive hard spheres, where preference for FCC over HCP polymorphs is weak, activity causes the annealing of HCP stacking faults, thus strongly favouring the FCC symmetry at high $Pe$. When freezing occurs more slowly, in the nucleation and growth regime, this tendency is much reduced and we see a trend towards the passive case of little preference for either polymorph.

cond-mat.soft↗

arXiv2021

Dynamics and Interactions of Quincke Roller Clusters: from Orbits and Flips to Excited States

Active matter systems may be characterised by the conversion of energy into active motion, e.g. the self-propulsion of microorganisms. Artificial active colloids form models which exhibit essential properties of more complex biological systems but are amenable to laboratory experiments. While most experimental models consist of spheres, such as Janus particles, active particles of different shapes are less understood. In particular, interactions between such active colloidal "molecules" are largely unexplored. Here, we investigate the motion of active colloidal molecules and the interactions between them. We focus on self-assembled dumbbells and trimers powered by an external electric field. For dumbbells, we observe an activity-dependent behaviour of spinning, circular and orbital motion. Moreover, collisions between dumbbells lead to the hierarchical self-assembly of tetramers and hexamers, both of which form rotational excited states. On the other hand, trimers exhibit a novel type of flipping motion that leads to trajectories reminiscent of a honeycomb lattice.

cond-mat.soft↗

arXiv2021

Protein-Polymer Mixtures in the Colloid Limit: Aggregation, Sedimentation and Crystallization

While proteins have been treated as particles with a spherically symmetric interaction, of course in reality the situation is rather more complex. A simple step towards higher complexity is to treat the proteins as non--spherical particles and that is the approach we pursue here. We investigate the phase behavior of enhanced green fluorescent protein (eGFP) under the addition of a non--adsorbing polymer, polyethylene glycol (PEG). From small angle x-ray scattering we infer that the eGFP undergoes dimerization and we treat the dimers as spherocylinders with aspect ratio $L/D-1 = 1.05$. Despite the complex nature of the proteins, we find that the phase behaviour is similar to that of hard spherocylinders with ideal polymer depletant, exhibiting aggregation and, in a small region of the phase diagram, crystallization. By comparing our measurements of the onset of aggregation with predictions for hard colloids and ideal polymers [S.V. Savenko and M. Dijkstra, J. Chem. Phys 124, 234902 (2006) and F. lo Verso et al., Phys. Rev. E 73, 061407 (2006)] we find good agreement, which suggests that the eGFP proteins are consistent with hard spherocylinders and ideal polymer.

cond-mat.soft↗

arXiv2021

Real Space Analysis of Colloidal Gels: Triumphs, Challenges and Future Directions

Colloidal gels constitute an important class of materials found in many contexts and with a wide range of applications. Yet as matter far from equilibrium, gels exhibit a variety of time-dependent behaviours, which can be perplexing, such as an increase in strength prior to catastrophic failure. Remarkably, such complex phenomena are faithfully captured by an extremely simple model - "sticky spheres". Here we review progress in our understanding of colloidal gels made through the use of real space analysis and particle resolved studies. We consider the challenges of obtaining a suitable experimental system where the refractive index and density of the colloidal particles is matched to that of the solvent. We review work to obtain a particle-level mechanism for rigidity in gels and the evolution of our understanding of time-dependent behaviour, from early-time aggregation to ageing, before considering the response of colloidal gels to deformation and then move on to more complex systems of anisotropic particles and mixtures. Finally we note some more exotic materials with similar properties.

cond-mat.soft↗

arXiv2021

Efficacy of face coverings in reducing transmission of COVID-19: calculations based on models of droplet capture

In the COVID--19 pandemic, among the more controversial issues is the use of masks and face coverings. Much of the concern boils down to the question -- just how effective are face coverings? One means to address this question is to review our understanding of the physical mechanisms by which masks and coverings operate -- steric interception, inertial impaction, diffusion and electrostatic capture. We enquire as to what extent these can be used to predict the efficacy of coverings. We combine the predictions of the models of these mechanisms which exist in the filtration literature and compare the predictions with recent experiments and lattice Boltzmann simulations, and find reasonable agreement with the former and good agreement with the latter. Building on these results, we explore the parameter space for woven cotton fabrics to show that three-layered cloth masks can be constructed with comparable filtration performance to surgical masks under ideal conditions. Reusable cloth masks thus present an environmentally friendly alternative to surgical masks so long as the face seal is adequate enough to minimise leakage.

cond-mat.soft↗

arXiv2021

Relaxation mechanisms in supercooled liquids past the Mode--Coupling Crossover: Cooperatively Re--arranging Regions vs Excitations

Among the challenges in discriminating between theoretical approaches to the glass transition is obtaining suitable data. In particular, particle--resolved data in liquids supercooled past the mode--coupling crossover has until recently been hard to obtain. Here we combine nano-particle resolved experiments and GPU simulation data which addresses this and investigate the predictions of differing theoretical approaches. We find support for both dynamic facilitation and thermodynamic approaches. In particular, excitations, the elementary units of relaxation in dynamic facilitation theory follow the predicted scaling behaviour and the properties of cooperatively rearranging regions (CRRs) are consistent with RFOT theory. At weak supercooling there is limited correlation between particles identified in excitations and CRRs, but this increases very substantially at deep supercooling. We identify a timescale related to the CRRs which is coupled to the structural relaxation time and thus decoupled from the excitation timescale, which remains microscopic.

cond-mat.soft↗

arXiv2021

Isomorphs in nanoconfined liquids

We study in this paper the possible existence of Roskilde-simple liquids and their isomorphs in a rough-wall nanoconfinement. Isomorphs are curves in the thermodynamic phase diagram along which structure and dynamics are invariant in suitable nondimensionalized units. Two model liquids using molecular dynamics computer simulations are considered: the single-component Lennard-Jones (LJ) liquid and the Kob-Andersen binary LJ mixture, both of which in the bulk phases are known to have isomorphs. Nanoconfinement is implemented by adopting a slit-pore geometry with fcc crystalline walls; this implies inhomogenous density profiles both parallel and perpendicular to the confining walls. Despite this fact and consistent with an earlier study [Ingebrigtsen et. al, Phys. Rev. Lett. 111, 235901 (2013)] we find that these nanoconfined liquids have isomorphs to a good approximation. More specifically, we show good scaling of inhomogenous density profiles, mean-square displacements, and higher-order structures probed using the topological cluster classification algorithm along the isomorphs. From this study, we conjecture that in experiments, Roskilde-simple liquids may exhibit isomorphs if confined in a suitable manner, for example with carbon nanotubes. Our study thus provides an alternative framework for understanding nanoconfined liquids.

cond-mat.soft↗

arXiv2020

Flexible confinement leads to multiple relaxation regimes in glassy colloidal liquids

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.

cond-mat.soft↗

arXiv2020

Active Dipolar Colloids in Three Dimensions: Strings, Sheets, Labyrinthine Textures and Crystals

Active matter exhibits striking behaviour reminiscent of living matter and molecular fluids, and has promising applications in drug delivery or mixing at the micron scale. Active colloidal systems provide important models with simple and controllable interactions amenable to theory and computer simulation. Experimental work is dominated by (quasi) two--dimensional (2d) systems at relatively low concentration, and rather less is known of the 3d case at concentrations pertinent to motility induced phase separation or to mimic morphogenesis. Here we investigate a 3d experimental system of active colloids in a dense suspension up to volume fractions of 0.5. The particles in our system are self-propelled in the lateral plane under an AC electric field. The field in addition induces an electric dipole, and the competition between activity and both steric and dipolar interactions gives rise to phase behaviour ranging from an active gas to a dynamic labyrinthine phase as well as dense tetragonal and hexagonal crystals. Intermediate volume fractions are characterised by two--dimensional sheets with large fluctuations reminiscent of active membranes. These active sheets break symmetry in a direction perpendicular to the applied field. Moreover, the relationship between electric field and the particle dynamics depends in a complex and unexpected manner upon the position in the state diagram.

cond-mat.soft↗