Transition from a simple yield stress fluid to a thixotropic material

From MRI rheometry we show that a pure emulsion can be turned from a simple yield stress fluid to a thixotropic material by adding a small fraction of colloidal particles. The two fluids have the same behavior in the liquid regime but the loaded emulsion exhibits a critical shear rate below which no steady flows can be observed. For a stress below the yield stress, the pure emulsion abruptly stops flowing, whereas the viscosity of the loaded emulsion continuously increases in time, which leads to an apparent flow stoppage. This phenomenon can be very well represented by a model assuming a progressive increase of the number of droplet links via colloidal particles.Comment: Published in Physical Review E. http://pre.aps.org/abstract/PRE/v76/i5/e05140

Bottlenecks to vibrational energy flow in OCS: Structures and mechanisms

Finding the causes for the nonstatistical vibrational energy relaxation in the planar carbonyl sulfide (OCS) molecule is a longstanding problem in chemical physics: Not only is the relaxation incomplete long past the predicted statistical relaxation time, but it also consists of a sequence of abrupt transitions between long-lived regions of localized energy modes. We report on the phase space bottlenecks responsible for this slow and uneven vibrational energy flow in this Hamiltonian system with three degrees of freedom. They belong to a particular class of two-dimensional invariant tori which are organized around elliptic periodic orbits. We relate the trapping and transition mechanisms with the linear stability of these structures.Comment: 13 pages, 13 figure

Self-learning Kinetic Monte-Carlo method: application to Cu(111)

We present a novel way of performing kinetic Monte Carlo simulations which does not require an {\it a priori} list of diffusion processes and their associated energetics and reaction rates. Rather, at any time during the simulation, energetics for all possible (single or multi-atom) processes, within a specific interaction range, are either computed accurately using a saddle point search procedure, or retrieved from a database in which previously encountered processes are stored. This self-learning procedure enhances the speed of the simulations along with a substantial gain in reliability because of the inclusion of many-particle processes. Accompanying results from the application of the method to the case of two-dimensional Cu adatom-cluster diffusion and coalescence on Cu(111) with detailed statistics of involved atomistic processes and contributing diffusion coefficients attest to the suitability of the method for the purpose.Comment: 18 pages, 9 figure

Thermonuclear burn-up in deuterated methane CD4CD_4

The thermonuclear burn-up of highly compressed deuterated methane CD$_4$ is considered in the spherical geometry. The minimal required values of the burn-up parameter $x = \rho_0 \cdot r_f$ are determined for various temperatures $T$ and densities $\rho_0$. It is shown that thermonuclear burn-up in $CD_4$ becomes possible in practice if its initial density $\rho_0$ exceeds $\approx 5 \cdot 10^3$ $g \cdot cm^{-3}$. Burn-up in CD$_2$T$_2$ methane requires significantly ($\approx$ 100 times) lower compressions. The developed approach can be used in order to compute the critical burn-up parameters in an arbitrary deuterium containing fuel

Deformation and flow of a two-dimensional foam under continuous shear

We investigate the flow properties of a two-dimensional aqueous foam submitted to a quasistatic shear in a Couette geometry. A strong localization of the flow (shear banding) at the edge of the moving wall is evidenced, characterized by an exponential decay of the average tangential velocity. Moreover, the analysis of the rapid velocity fluctuations reveals self-similar dynamical structures consisting of clusters of bubbles rolling as rigid bodies. To relate the instantaneous (elastic) and time-averaged (plastic) components of the strain, we develop a stochastic model where irreversible rearrangements are activated by local stress fluctuations originating from the rubbing of the wall. This model gives a complete description of our observations and is also consistent with data obtained on granular shear bands by other groups.Comment: 5 pages, 2 figure

Surface diffusion coefficients by thermodynamic integration: Cu on Cu(100)

The rate of diffusion of a Cu adatom on the Cu(100) surface is calculated using thermodynamic integration within the transition state theory. The results are found to be in excellent agreement with the essentially exact values from molecular-dynamics simulations. The activation energy and related entropy are shown to be effectively independent of temperature, thus establishing the validity of the Arrhenius law over a wide range of temperatures. Our study demonstrates the equivalence of diffusion rates calculated using thermodynamic integration within the transition state theory and direct molecular-dynamics simulations.Comment: 4 pages (revtex), two figures (postscript

The Escape Problem for Irreversible Systems

The problem of noise-induced escape from a metastable state arises in physics, chemistry, biology, systems engineering, and other areas. The problem is well understood when the underlying dynamics of the system obey detailed balance. When this assumption fails many of the results of classical transition-rate theory no longer apply, and no general method exists for computing the weak-noise asymptotics of fundamental quantities such as the mean escape time. In this paper we present a general technique for analysing the weak-noise limit of a wide range of stochastically perturbed continuous-time nonlinear dynamical systems. We simplify the original problem, which involves solving a partial differential equation, into one in which only ordinary differential equations need be solved. This allows us to resolve some old issues for the case when detailed balance holds. When it does not hold, we show how the formula for the mean escape time asymptotics depends on the dynamics of the system along the most probable escape path. We also present new results on short-time behavior and discuss the possibility of focusing along the escape path.Comment: 24 pages, APS revtex macros (version 2.1) now available from PBB via `get oldrevtex.sty

A Scaling Theory of Bifurcations in the Symmetric Weak-Noise Escape Problem

We consider the overdamped limit of two-dimensional double well systems perturbed by weak noise. In the weak noise limit the most probable fluctuational path leading from either point attractor to the separatrix (the most probable escape path, or MPEP) must terminate on the saddle between the two wells. However, as the parameters of a symmetric double well system are varied, a unique MPEP may bifurcate into two equally likely MPEP's. At the bifurcation point in parameter space, the activation kinetics of the system become non-Arrhenius. In this paper we quantify the non-Arrhenius behavior of a system at the bifurcation point, by using the Maslov-WKB method to construct an approximation to the quasistationary probability distribution of the system that is valid in a boundary layer near the separatrix. The approximation is a formal asymptotic solution of the Smoluchowski equation. Our analysis relies on the development of a new scaling theory, which yields `critical exponents' describing weak-noise behavior near the saddle, at the bifurcation point.Comment: LaTeX, 60 pages, 24 Postscript figures. Uses epsf macros to include the figures. A file in `uufiles' format containing the figures is separately available at ftp://platinum.math.arizona.edu/pub/papers-rsm/paperF/figures.uu and a Postscript version of the whole paper (figures included) is available at ftp://platinum.math.arizona.edu/pub/papers-rsm/paperF/paperF.p