Searcharxiv⌕ Search

arXiv subjects

R. M. L. Evans

Publications and source records attributed to R. M. L. Evans.

At least 19 recordsLinked to original sources

Effects of orientational order on modulated cylindrical interfaces

Cylindrical interfaces occur in sheared or deformed emulsions and as biological or technological lipid monolayer or bilayer tubules. Like the corresponding spherical droplets and vesicles, these cylinder-like surfaces may host orientaional order with $n$-fold rotational symmetry, for example in the positions of lipid molecules or of spherical nanoparticles. We examine how that order interacts with and induces shape modulations of cylindrical interfaces. While on spherical droplets $2n$ topological defects necessarily exist and can induce icosahedral droplet shapes, the cylindrical topology is compatible with a defect-free patterning. Nevertheless, once a modulation is introduced by a mechanism such as spontaneous curvature, nontrivial patterns of order, including ones with excess defects, emerge and have nonlinear effects on the shape of the tube. Examining the equilibrium energetics of the system analytically and with a lattice-based Markov chain Monte Carlo simulation, we predict low-temperature morphologies of modulated cylindrical interfaces hosting orientational order. A shape modulation induces a banded pattern of alternatingly isotropic and ordered interfacial material. Furthermore cylindrical systems can be divided into Type I, without defects, and Type II, which go through a spectrum of defect states with up to $4n$ excess defects. The character of the curvature-induced shape transition from unmodulated to modulated cylinders is continuous or discontinuous accordingly.

cond-mat.soft↗

The simplest microscopic model of a complex fluid: flow phenomena and constitutive relation

It was shown in [PRL 114, 138301 (2015)] that a remarkably simple dynamical model exhibits many of the complex flow regimes and non-equilibrium phase transitions characteristic of complex fluids. By removing extraneous detail, this simplest microscopic model of non-Newtonian flow can reveal the universal physics relevant to all complex fluids. Here we present more detailed results and a full derivation of the model's compact mean-field constitutive relation, with great potential scope for insights into universality and tractable mathematics. By enforcing local conservation of angular momentum, the one-dimensional (1D) XY-model (originally used for equilibrium magnetic systems) can be driven into various flow regimes, including simple Newtonian behaviour, shear banding, solid-liquid coexistence and slip-plane motion. The model demonstrates that the phenomenon of shear banding does not rely on details of tensorial stress fields, but can exist in 1D.

cond-mat.soft↗

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↗

Numerical comparison of a constrained path ensemble and a driven quasisteady state

We investigate the correspondence between a non-equilibrium ensemble defined via the distribution of phase-space paths of a Hamiltonian system, and a system driven into a steady-state by non-equilibrium boundary conditions. To discover whether the non-equilibrium path ensemble adequately describes the physics of a driven system, we measure transition rates in a simple one-dimensional model of rotors with Newtonian dynamics and purely conservative interactions. We compare those rates with known properties of the non-equilibrium path ensemble. In doing so, we establish effective protocols for the analysis of transition rates in non-equilibrium quasi-steady states. Transition rates between potential wells and also between phase-space elements are studied, and found to exhibit distinct properties, the more coarse-grained potential wells being effectively further from equilibrium. In all cases the results from the boundary-driven system are close to the path-ensemble predictions, but the question of equivalence of the two remains open.

cond-mat.stat-mech↗

Optical tweezers: wideband microrheology

Microrheology is a branch of rheology having the same principles as conventional bulk rheology, but working on micron length scales and micro-litre volumes. Optical tweezers have been successfully used with Newtonian fluids for rheological purposes such as determining fluid viscosity. Conversely, when optical tweezers are used to measure the viscoelastic properties of complex fluids the results are either limited to the material's high-frequency response, discarding important information related to the low-frequency behavior, or they are supplemented by low-frequency measurements performed with different techniques, often without presenting an overlapping region of clear agreement between the sets of results. We present a simple experimental procedure to perform microrheological measurements over the widest frequency range possible with optical tweezers. A generalised Langevin equation is used to relate the frequency-dependent moduli of the complex fluid to the time-dependent trajectory of a probe particle as it flips between two optical traps that alternately switch on and off.

physics.optics↗

Comment on `Detailed balance has a counterpart in non-equilibrium steady states'

Transition rates in continuously driven steady states were derived in [Evans R M L, 2005 J. Phys. A: Math. Gen. 38, 293] by demanding that no information other than the microscopic laws of motion and the macroscopic observables of the system be used to describe it. In addition to the mean energy at equilibrium, and unlike them, these driven states have a finite throughput of flux. This implies that the (nonequilibrium) reservoir, to which the system is weakly coupled, is fully characterised by its mean energy and mean flux. While we expect the resulting prescription for the rates in continuous and discretised time versions of models of real systems to be equivalent, it is not trivial to see this from the expression for the rates derived previously. We demonstrate this equivalence for a model of activated processes solved previously for continuous time, thus demonstrating consistency of theory.

cond-mat.stat-mech↗

Nonequilibrium statistical mechanics of shear flow: invariant quantities and current relations

In modeling nonequilibrium systems one usually starts with a definition of the microscopic dynamics, e.g., in terms of transition rates, and then derives the resulting macroscopic behavior. We address the inverse question for a class of steady state systems, namely complex fluids under continuous shear flow: how does an externally imposed shear current affect the microscopic dynamics of the fluid? The answer can be formulated in the form of invariant quantities, exact relations for the transition rates in the nonequilibrium steady state, as discussed in a recent letter [A. Baule and R. M. L. Evans, Phys. Rev. Lett. 101, 240601 (2008)]. Here, we present a more pedagogical account of the invariant quantities and the theory underlying them, known as the nonequilibrium counterpart to detailed balance (NCDB). Furthermore, we investigate the relationship between the transition rates and the shear current in the steady state. We show that a fluctuation relation of the Gallavotti-Cohen type holds for systems satisfying NCDB.

cond-mat.stat-mech↗

Statistical mechanics far from equilibrium: prediction and test for a sheared system

We report the complete statistical treatment of a system of particles interacting via Newtonian forces in continuous boundary-driven flow, far from equilibrium. By numerically time-stepping the force-balance equations of a model fluid we measure occupancies and transition rates in simulation. The high-shear-rate simulation data verify the invariant quantities predicted by our statistical theory, thus demonstrating that a class of non-equilibrium steady states of matter, namely sheared complex fluids, is amenable to statistical treatment from first principles.

cond-mat.stat-mech↗

Measuring storage and loss moduli using optical tweezers: broadband microrheology

We present an experimental procedure to perform broadband microrheological measurements with optical tweezers. A generalised Langevin equation is adopted to relate the time-dependent trajectory of a particle in an imposed flow to the frequency-dependent moduli of the complex fluid. This procedure allows us to measure the material linear viscoelastic properties across the widest frequency range achievable with optical tweezers.

cond-mat.soft↗

Dynamics of semi-flexible polymer solutions in the highly entangled regime

We present experimental evidence that the effective medium approximation (EMA), developed by D.C. Morse [Phys. Rev. E {\bf 63}, 031502, (2001)], provides the correct scaling law of the macroscopic plateau modulus $G^{0}\proptoρ^{4/3}L^{-1/3}_{p}$ (where $ρ$ is the contour length per unit volume and $L_{p}$ is the persistence length) of semi-flexible polymer solutions, in the highly entangled concentration regime. Competing theories, including a self-consistent binary collision approximation (BCA), have instead predicted $G^{0}\proptoρ^{7/5}L^{-1/5}_{p}$. We have tested both the EMA and BCA scaling predictions using actin filament (F-actin) solutions which permit experimental control of $L_p$ independently of other parameters. A combination of passive video particle tracking microrheology and dynamic light scattering yields independent measurements of the elastic modulus $G$ and $L_{p}$ respectively. Thus we can distinguish between the two proposed laws, in contrast to previous experimental studies, which focus on the (less discriminating) concentration functionality of $G$.

cond-mat.soft↗

Invariant quantities in shear flow

The dynamics of systems out of thermal equilibrium is usually treated on a case-by-case basis without knowledge of fundamental and universal principles. We address this problem for a class of driven steady states, namely those mechanically driven at the boundaries such as complex fluids under shear. From a nonequilibrium counterpart to detailed balance (NCDB) we derive a remarkably simple set of invariant quantities which remain unchanged when the system is driven. These new nonequilibrium relations are both exact and valid arbitrarily far from equilibrium. Furthermore, they enable the systematic calculation of transition rates in driven systems with state-spaces of arbitrary connectivity.

cond-mat.stat-mech↗

Validation of the Jarzynski relation for a system with strong thermal coupling: an isothermal ideal gas model

We revisit the paradigm of an ideal gas under isothermal conditions. A moving piston performs work on an ideal gas in a container that is strongly coupled to a heat reservoir. The thermal coupling is modelled by stochastic scattering at the boundaries. In contrast to recent studies of an adiabatic ideal gas with a piston [R.C. Lua and A.Y. Grosberg, \textit{J. Phys. Chem. B} 109, 6805 (2005); I. Bena et al., \textit{Europhys. Lett.} 71, 879 (2005)], container and piston stay in contact with the heat bath during the work process. Under this condition the heat reservoir as well as the system depend on the work parameter $λ$ and microscopic reversibility is broken for a moving piston. Our model is thus not included in the class of systems for which the non-equilibrium work theorem has been derived rigorously either by Hamiltonian [C. Jarzynski, \textit{J. Stat. Mech.} P09005 (2004)] or stochastic methods [G.E. Crooks, \textit{J. Stat. Phys.} 90, 1481 (1998)]. Nevertheless the validity of the non-equilibrium work theorem is confirmed both numerically for a wide range of parameter values and analytically in the limit of a very fast moving piston, i.e. in the far non-equilibrium regime.

cond-mat.stat-mech↗

Properties of a non-equilibrium heat bath

At equilibrium, a fluid element, within a larger heat bath, receives random impulses from the bath. Those impulses, which induce stochastic transitions in the system (the fluid element), respect the principle of detailed balance, because the bath is also at equilibrium. Under continuous shear, the fluid element adopts a non-equilibrium steady state. Because the surrounding bath of fluid under shear is also in a non-equilibrium steady state, the system receives stochastic impulses with a non-equilibrium distribution. Those impulses no longer respect detailed balance, but are nevertheless constrained by rules. The rules in question, which are applicable to a wide sub-class of driven steady states, were recently derived [R. M. L. Evans, Phys. Rev. Lett. {\bf 92}, 150601 (2004); J. Phys. A: Math. Gen. {\bf 38}, 293 (2005)] using information-theoretic arguments. In the present paper, we provide a more fundamental derivation, based on the uncontroversial, non-Bayesian interpretation of probabilities as simple ratios of countable quantities. We apply the results to some simple models of interacting particles, to investigate the nature of forces that are mediated by a non-equilibrium noise-source such as a fluid under shear.

cond-mat.stat-mech↗

Detailed balance has a counterpart in non-equilibrium steady states

When modelling driven steady states of matter, it is common practice either to choose transition rates arbitrarily, or to assume that the principle of detailed balance remains valid away from equilibrium. Neither of those practices is theoretically well founded. Hypothesising ergodicity constrains the transition rates in driven steady states to respect relations analogous to, but different from the equilibrium principle of detailed balance. The constraints arise from demanding that the design of any model system contains no information extraneous to the microscopic laws of motion and the macroscopic observables. This prevents over-description of the non-equilibrium reservoir, and implies that not all stochastic equations of motion are equally valid. The resulting recipe for transition rates has many features in common with equilibrium statistical mechanics.

cond-mat.stat-mech↗

Rules for transition rates in nonequilibrium steady states

Just as transition rates in a canonical ensemble must respect the principle of detailed balance, constraints exist on transition rates in driven steady states. I derive those constraints, by maximum information-entropy inference, and apply them to the steady states of driven diffusion and a sheared lattice fluid. The resulting ensemble can potentially explain nonequilibrium phase behaviour and, for steady shear, gives rise to stress-mediated long-range interactions.

cond-mat.stat-mech↗

Correlation length by measuring empty space in simulated aggregates

We examine the geometry of the spaces between particles in diffusion-limited cluster aggregation, a numerical model of aggregating suspensions. Computing the distribution of distances from each point to the nearest particle, we show that it has a scaled form independent of the concentration phi, for both two- (2D) and three-dimensional (3D) model gels at low phi. The mean remoteness is proportional to the density-density correlation length of the gel, xi, allowing a more precise measurement of xi than by other methods. A simple analytical form for the scaled remoteness distribution is developed, highlighting the geometrical information content of the data. We show that the second moment of the distribution gives a useful estimate of the permeability of porous media.

cond-mat.stat-mech↗

Diffusive growth of polydisperse hard-sphere crystals

Unlike atoms, colloidal particles are not identical, but can only be synthesised within a finite size tolerance. Colloids are therefore polydisperse, i.e. mixtures of infinitely many components with sizes drawn from a continuous distribution. We model the crystallisation of hard-sphere colloids (with/without attractions) from an initially amorphous phase. Though the polydisperse hard-sphere phase diagram has been widely studied, it is not straightforwardly applicable to real colloidal crystals, since they are inevitably out of equilibrium. The process by which colloidal crystals form determines the size distribution of the particles that comprise them. Once frozen into the crystal lattice, the particles are caged so that the composition cannot subsequently relax to the equilibrium optimum. We predict that the mean size of colloidal particles incorporated into a crystal is smaller than anticipated by equilibrium calculations. This is because small particles diffuse fastest and therefore arrive at the crystal in disproportionate abundance.

cond-mat.soft↗

Perturbative polydispersity: Phase equilibria of near-monodisperse systems

The conditions of multi-phase equilibrium are solved for generic polydisperse systems. The case of multiple polydispersity is treated, where several properties (e.g. size, charge, shape) simultaneously vary from one particle to another. By developing a perturbative expansion in the width of the distribution of constituent species, it is possible to calculate the effects of polydispersity alone, avoiding difficulties associated with the underlying many-body problem. Explicit formulae are derived in detail, for the partitioning of species at coexistence and for the shift of phase boundaries due to polydispersity. `Convective fractionation' is quantified, whereby one property (e.g. charge) is partitioned between phases due to a driving force on another. To demonstrate the ease of use and versatility of the formulae, they are applied to models of a chemically-polydisperse polymer blend, and of fluid-fluid coexistence in polydisperse colloid-polymer mixtures. In each case, the regime of coexistence is shown to be enlarged by polydispersity.

cond-mat.stat-mech↗