arXiv subjects

Christopher J. Fullerton

Publications and source records attributed to Christopher J. Fullerton.

10 recordsLinked to original sources

arXiv2020

Glassy behaviour of sticky spheres: What lies beyond experimental timescales?

We use the swap Monte Carlo algorithm to analyse the glassy behaviour of sticky spheres in equilibrium conditions at densities where conventional simulations and experiments fail to reach equilibrium, beyond predicted phase transitions and dynamic singularities. We demonstrate the existence of a unique ergodic region comprising all the distinct phases previously reported, except for a phase-separated region at strong adhesion. All structural and dynamic observables evolve gradually within this ergodic region, the physics evolving smoothly from well-known hard sphere glassy behaviour at small adhesions and large densities, to a more complex glassy regime characterised by unusually-broad distributions of relaxation timescales and lengthscales at large adhesions.

cond-mat.soft↗

arXiv2019

Front-mediated melting of ultrastable glasses

Ultrastable vapor-deposited glasses display uncommon material properties. Most remarkably, upon heating they are believed to melt via a liquid front that originates at the free surface and propagates over a mesoscopic crossover length, before crossing over to bulk melting. We combine swap Monte Carlo with molecular dynamics simulations to prepare and melt isotropic amorphous films of unprecedendtly high kinetic stability. We are able to directly observe both bulk and front melting, and the crossover between them. We measure the front velocity over a broad range of conditions, and a crossover length scale that grows to nearly $400$ particle diameters in the regime accessible to simulations. Our results disentangle the relative roles of kinetic stability and vapor deposition in the physical properties of stable glasses.

cond-mat.soft↗

arXiv2018

Efficient swap algorithms for molecular dynamics simulations of equilibrium supercooled liquids

It was recently demonstrated that a simple Monte Carlo (MC) algorithm involving the swap of particle pairs dramatically accelerates the equilibrium sampling of simulated supercooled liquids. We propose two numerical schemes integrating the efficiency of particle swaps into equilibrium molecular dynamics (MD) simulations. We first develop a hybrid MD/MC scheme combining molecular dynamics with the original swap Monte Carlo. We implement this hybrid method in LAMMPS, a software package employed by a large community of users. Secondly, we define a continuous time version of the swap algorithm where both the positions and diameters of the particles evolve via Hamilton's equations of motion. For both algorithms, we discuss in detail various technical issues as well as the optimisation of simulation parameters. We compare the numerical efficiency of all available swap algorithms and discuss their relative merits.

cond-mat.stat-mech↗

arXiv2017

Density controls the kinetic stability of ultrastable glasses

We use a swap Monte Carlo algorithm to numerically prepare bulk glasses with kinetic stability comparable to that of glass films produced experimentally by physical vapor deposition. By melting these systems into the liquid state, we show that some of our glasses retain their amorphous structures longer than 10^5 times the equilibrium structural relaxation time. This exceptional kinetic stability cannot be achieved experimentally for bulk materials. We perform simulations at both constant volume and constant pressure to demonstrate that the density mismatch between the ultrastable glass and the equilibrium liquid accounts for a major part of the observed kinetic stability.

cond-mat.soft↗

arXiv2017

Effects of vertical confinement on gelation and sedimentation of colloids

We consider the sedimentation of a colloidal gel under confinement in the direction of gravity. The confinement allows us to compare directly experiments and computer simulations, for the same system size in the vertical direction. The confinement also leads to qualitatively different behaviour compared to bulk systems: in large systems gelation suppresses sedimentation, but for small systems sedimentation is enhanced relative to non-gelling suspensions, although the rate of sedimentation is reduced when the strength of the attraction between the colloids is strong. We map interaction parameters between a model experimental system (observed in real space) and computer simulations. Remarkably, we find that when simulating the system using Brownian dynamics in which hydrodynamic interactions between the particles are neglected, we find that sedimentation occurs on the same timescale as the experiments, however the thickness of the "arms" of the gel is rather larger in the experiments, compared with the simulations. An analysis of local structure in the simulations showed similar behaviour to gelation in the absence of gravity.

cond-mat.soft↗

arXiv2016

Optimising self-assembly through time-dependent interactions

We demonstrate a simple method by which time-dependent interactions can be exploited to improve self-assembly in colloidal systems. We apply this method to two systems: a model colloid with short-ranged attractive potentials that undergoes crystallisation, and a schematic model of cluster growth. The method is based on initially strong bonds between particles, to accelerate nucleation, followed by a stage with weaker bonds, to promote growth of high-quality assembled structures. We track the growth of clusters during assembly, which reveals insight into effects of multiple nucleation events, and of competition between the growth of clusters with different properties.

cond-mat.soft↗

arXiv2013

Investigating amorphous order in stable glasses by random pinning

We use a random pinning procedure to investigate stable glassy states associated with large deviations of the activity in a model glass-former. We pin particles both from active (equilibrium) configurations and from stable (inactive) glassy states. By comparing the distribution of the overlap between states that share pinned particles, we infer that the inactive states are characterised by a structural length scale that is comparable with the system size. This is a manifestation of amorphous order in these glassy states, which helps to explain their stability.

cond-mat.stat-mech↗

arXiv2013

Dynamical correlations in a glass-former with randomly pinned particles

The effects of randomly pinning particles in a model glass-forming fluid are studied, with a focus on the dynamically heterogeneous relaxation in the presence of pinning. We show how four-point dynamical correlations can be analysed in real space, allowing direct extraction of a length scale that characterises dynamical heterogeneity. In the presence of pinning, the relaxation time of the glassy system increases by up to two decades, but there is almost no increase in either the four-point correlation length or the strength of the four-point correlations. We discuss the implications of these results for theories of the glass transition.

cond-mat.stat-mech↗

arXiv2013

The Growing Correlation Length in Glasses

The growing correlation length observed in supercooled liquids as their temperature is lowered has been studied with the aid of a single occupancy cell model. This model becomes more accurate as the density of the system is increased. One of its advantages is that it permits a simple mapping to a spin system and the effective spin Hamiltonian is easily obtained for smooth interparticle potentials. For a binary liquid mixture the effective spin Hamiltonian is in the universality class of the Ising spin glass in a field. No phase transition at finite temperatures is therefore expected and the correlation length will stay finite right down to zero temperature. For binary mixtures of hard disks and spheres we were not able to obtain the effective spin Hamiltonian analytically, but have done simulations to obtain its form. It again is in the universality class of the Ising spin glass in a field. However, in this case the effective field can be shown to go to zero at the density of maximum packing in the model, (which is close to that of random close packing), which means that the correlation length will diverge as the density approaches its maximum. The exponent nu describing the divergence is related in d dimensions to the Ising spin glass domain wall energy exponent theta.

cond-mat.stat-mech↗

arXiv2013

Dynamical phase transitions in supercooled liquids: interpreting measurements of dynamical activity

We study dynamical phase transitions in a model supercooled liquid. These transitions occur in ensembles of trajectories that are biased towards low (or high) dynamical activity. We compare two different measures of activity that were introduced in recent papers and we find that they are anti-correlated with each other. To interpret this result, we show that the two measures couple to motion on different length and time scales. We find that inactive states with very slow structural relaxation nevertheless have increased molecular motion on short scales. We discuss these results in terms of the potential energy landscape of the system and in terms of the liquid structure in active/inactive states.

cond-mat.stat-mech↗