arXiv subjects

Robert L. Jack

Publications and source records attributed to Robert L. Jack.

At least 91 records · Page 5Linked to original sources

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↗

arXiv2016

Coarse-grained depletion potentials for anisotropic colloids: application to lock-and-key systems

When a colloid is mixed with a depletant such as a non-adsorbing polymer, one observes attractive effective interactions between the colloidal particles. If these particles are anisotropic, analysis of these effective interactions is challenging in general. We present a method for inference of approximate (coarse-grained) effective interaction potentials between such anisotropic particles. Using the example of indented (lock-and-key) colloids, we show how numerical solutions can be used to integrate out the (hard sphere) depletant, leading to a depletion potential that accurately characterises the effective interactions. The accuracy of the method is based on matching of contributions to the second virial coefficient of the colloids. The simplest version of our method yields a piecewise-constant effective potential; we also show how this scheme can be generalised to other functional forms, where appropriate.

cond-mat.soft↗

arXiv2016

Structure of inactive states of a binary Lennard-Jones mixture

We study the structure of inactive states in a prototypical model glass, the Kob-Andersen binary Lennard-Jones mixture. These inactive states are obtained by transition path sampling and are at dynamical phase coexistence with an active equilibrium state. Configurations in the inactive states are kinetically stable and are located in deeper basins of the energy landscape than their active counterparts. By analyzing trajectory-to-trajectory fluctuations within the inactive state, we assess correlations between kinetic stability, energy and other structural properties. We show that measures of local order associated to stable local packings and bond-orientational order are weakly correlated with energy and kinetic stability. We discuss what kinds of structural measurement might capture the relevant dynamical features of the inactive state.

cond-mat.stat-mech↗

arXiv2016

Population dynamics method with a multi-canonical feedback control

We discuss the Giardinà-Kurchan-Peliti population dynamics method for evaluating large deviations of time averaged quantities in Markov processes [Phys. Rev. Lett. \textbf{96}, 120603 (2006)]. This method exhibits systematic errors which can be large in some circumstances, particularly for systems with weak noise, with many degrees of freedom, or close to dynamical phase transitions. We show how these errors can be mitigated by introducing control forces within the algorithm. These forces are determined by an iteration-and-feedback scheme, inspired by multicanonical methods in equilibrium sampling. We demonstrate substantially improved results in a simple model and we discuss potential applications to more complex systems.

cond-mat.stat-mech↗

arXiv2016

Ideal bulk pressure of active Brownian particles

The extent to which active matter might be described by effective equilibrium concepts like temperature and pressure is currently being discussed intensely. Here we study the simplest model, an ideal gas of non-interacting active Brownian particles. While the mechanical pressure exerted onto confining walls has been linked to correlations between particles' positions and their orientations, we show that these correlations are entirely controlled by boundary effects. We also consider a definition of local pressure, which describes interparticle forces in terms of momentum exchange between different regions of the system. We present three pieces of analytical evidence which indicate that such a local pressure exists, and we show that its bulk value differs from the mechanical pressure exerted on the walls of the system. We attribute this difference to the fact that the local pressure in the bulk does not depend on boundary effects, contrary to the mechanical pressure. We carefully examine these boundary effects using a channel geometry, and we show a virial formula for the pressure correctly predicts the mechanical pressure even in finite channels. However, this result no longer holds in more complex geometries, as exemplified for a channel that includes circular obstacles.

cond-mat.stat-mech↗

arXiv2016

The melting of stable glasses is governed by nucleation-and-growth dynamics

We discuss the microscopic mechanisms by which low-temperature amorphous states, such as ultrastable glasses, transform into equilibrium fluids, after a sudden temperature increase. Experiments suggest that this process is similar to the melting of crystals, thus differing from the behaviour found in ordinary glasses. We rationalize these observations using the physical idea that the transformation process takes place very close to a `hidden' equilibrium first-order phase transition, which is observed in systems of coupled replicas. We illustrate our views using simulation results for a simple two-dimensional plaquette spin model, which is known to exhibit a range of glassy behaviour. Our results suggest that nucleation-and-growth dynamics, as found near ordinary first-order transitions, is also the correct theoretical framework to analyse the melting of ultrastable glasses. Our approach provides a unified understanding of multiple experimental observations, such as propagating melting fronts, large kinetic stability ratios, and `giant' dynamic lengthscales.

cond-mat.stat-mech↗

arXiv2016

Absence of dissipation in trajectory ensembles biased by currents

We consider biased ensembles of trajectories associated with large deviations of currents in equilibrium systems. The biased ensembles are characterised by non-zero currents and lack the time-reversal symmetry of the equilibrium state, but we show that they retain a generalised time-reversal symmetry, involving a spatial transformation that inverts the current. This means that these ensembles lack dissipation. Hence, they differ significantly from non-equilibrium steady states where currents are induced by external forces. One consequence of this result is that maximum entropy assumptions (MaxEnt/MaxCal), widely used for modelling thermal systems away from equilibrium, have quite unexpected implications, including apparent superfluid behaviour in a classical model of shear flow.

cond-mat.stat-mech↗

arXiv2015

Phase transition for quenched coupled replicas in a plaquette spin model of glasses

We study a three-dimensional plaquette spin model whose low temperature dynamics is glassy, due to localised defects and effective kinetic constraints. While the thermodynamics of this system is smooth at all temperatures, we show that coupling it to a second system with a fixed (quenched) configuration can lead to a phase transition, at finite coupling. The order parameter is the overlap between the copies, and the transition is between phases of low and high overlap. We find critical points whose properties are consistent with random-field Ising universality. We analyse the interfacial free energy cost between the high- and low-overlap states that coexist at (and below) the critical point, and we use this cost as the basis for a finite-size scaling analysis. We discuss these results in the context of mean-field and dynamical facilitation theories of the glass transition.

cond-mat.stat-mech↗

arXiv2015

Dynamical phase transitions in one-dimensional hard-particle systems

We analyse a one-dimensional model of hard particles, within ensembles of trajectories that are conditioned (or biased) to atypical values of the time-averaged dynamical activity. We analyse two phenomena that are associated with these large deviations of the activity: phase separation (at low activity) and the formation of hyperuniform states (at high activity). We consider a version of the model which operates at constant volume, and a version at constant pressure. In these non-equilibrium systems, differences arise between the two ensembles, because of the extra freedom available to the constant-pressure system, which can change its total density. We discuss the relationships between different ensembles, mechanical equilibrium, and the probability cost of rare density fluctuations.

cond-mat.stat-mech↗

arXiv2015

Overlap and activity glass transitions in plaquette spin models with hierarchical dynamics

We consider thermodynamic and dynamic phase transitions in plaquette spin models of glasses. The thermodynamic transitions involve coupled (annealed) replicas of the model. We map these coupled-replica systems to a single replica in a magnetic field, which allows us to analyse the resulting phase transitions in detail. For the triangular plaquette model (TPM), we find for the coupled-replica system a phase transition between high- and low-overlap phases, occuring at a coupling eps*(T), which vanishes in the low-temperature limit. Using computational path sampling techniques, we show that a single TPM also displays space-time transitions between active and inactive dynamical phases. These first-order dynamical transitions occur at a critical counting field s_c(T)>=0 that appears to vanish at zero temperature, in a manner reminiscent of the thermodynamic overlap transition. In order to extend the ideas to three dimensions we introduce the square pyramid model which also displays both overlap and activity transitions. We discuss a possible common origin of these various phase transitions, based on long-lived (metastable) glassy states.

cond-mat.stat-mech↗

arXiv2015

Evidence for a disordered critical point in a glass-forming liquid

Using computer simulations of an atomistic glass-forming liquid, we investigate the fluctuations of the overlap between a fluid configuration and a quenched reference system. We find that large fluctuations of the overlap develop as temperature decreases, consistent with the existence of the random critical point that is predicted by effective field theories. We discuss the scaling of fluctuations near the presumed critical point, comparing the observed behaviour with that of the random-field Ising model. We argue that this critical point directly reveals the existence of an interfacial tension between amorphous metastable states, a quantity relevant both for equilibrium relaxation and for nonequilibrium melting of stable glass configurations.

cond-mat.stat-mech↗

arXiv2015

Unusual liquid phases for indented colloids with depletion interactions

We study indented spherical colloids, interacting via depletion forces. These systems exhibit liquid-vapor phase transitions whose properties are determined by a combination of strong "lock-and-key" bonds and weaker non-specific interactions. As the propensity for lock-and-key binding increases, the critical point moves to significantly lower density, and the coexisting phases change their structure. In particular, the liquid phase is "porous", exhibiting large percolating voids. The properties of this system depend strongly on the topological structure of an underlying bond network: we comment on the implications of this fact for the assembly of equilibrium states with controlled porous structures.

cond-mat.soft↗

arXiv2015

Effective interactions and large deviations in stochastic processes

We discuss the relationships between large deviations in stochastic systems, and "effective interactions" that induce particular rare events. We focus on the nature of these effective interactions in physical systems with many interacting degrees of freedom, which we illustrate by reviewing several recent studies. We describe the connections between effective interactions, large deviations at "level 2.5", and the theory of optimal control. Finally, we discuss possible physical applications of variational results associated with those theories.

cond-mat.stat-mech↗

arXiv2014

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↗

arXiv2014

The Statistical Mechanics of Dynamic Pathways to Self-assembly

We describe some of the important physical characteristics of the `pathways', i.e. dynamical processes, by which molecular, nanoscale and micron-scale self-assembly occurs. We highlight the fact that there exist features of self-assembly pathways that are common to a wide range of physical systems, even though those systems may be different in respect of their microscopic details. We summarize some existing theoretical descriptions of self-assembly pathways, and highlight areas -- notably, the description of self-assembly pathways that occur `far' from equilibrium -- that are likely to become increasingly important.

cond-mat.stat-mech↗

arXiv2014

Hyperuniformity and phase separation in biased ensembles of trajectories for diffusive systems

We analyse biased ensembles of trajectories for diffusive systems. In trajectories biased either by the total activity or the total current, we use fluctuating hydrodynamics to show that these systems exhibit phase transtions into `hyperuniform' states, where large-wavelength density fluctuations are strongly suppressed. We illustrate this behaviour numerically for a system of hard particles in one dimension and we discuss how it appears in simple exclusion processes. We argue that these diffusive systems generically respond very strongly to any non-zero bias, so that homogeneous states with "normal" fluctuations (finite compressibility) exist only when the bias is very weak.

cond-mat.stat-mech↗

arXiv2014

Geometrical interpretation of fluctuating hydrodynamics in diffusive systems

We discuss geometric formulations of hydrodynamic limits in diffusive systems. Specifically, we describe a geometrical construction in the space of density profiles --- the Wasserstein geometry --- which allows the deterministic hydrodynamic evolution of the systems to be related to steepest descent of the free energy, and show how this formulation can be related to most probable paths of mesoscopic dissipative systems. The geometric viewpoint is also linked to fluctuating hydrodynamics of these systems via a saddle point argument.

cond-mat.stat-mech↗

arXiv2014

Information-theoretic measurements of coupling between structure and dynamics in glass-formers

We analyse the connections between structure and dynamics in two model glass-formers, using the mutual information between an initial configuration and the ensuing dynamics to compare the predictive value of different structural observables. We consider the predictive power of normal modes, locally favoured structures, and coarse-grained measurements of local energy and density. The mutual information allows the influence of the liquid structure on the dynamics to be analysed quantitatively as a function of time, showing that normal modes give the most useful predictions on short time scales while local energy and density are most strongly predictive at long times.

cond-mat.stat-mech↗