Multiple jumps and vacancy diffusion in a face-centered cubic metal

The diffusion of monovacancies in gold has been studied by computer simulation. Multiple jumps have been found to play a central role in the atomic dynamics at high temperature, and have been shown to be responsible for an upward curvature in the Arrhenius plot of the diffusion coefficient. Appropriate saddle points on the potential energy surface have been found, supporting the interpretation of vacancy multiple jumps as distinct migration mechanisms.Comment: 16 page

Physicality and Cooperative Design

CSCW researchers have increasingly come to realize that material work setting and its population of artefacts play a crucial part in coordination of distributed or co-located work. This paper uses the notion of physicality as a basis to understand cooperative work. Using examples from an ongoing fieldwork on cooperative design practices, it provides a conceptual understanding of physicality and shows that material settings and co-worker’s working practices play an important role in understanding physicality of cooperative design

Crossover between hydrodynamic and kinetic modes in binary liquid alloys

Inelastic x-ray scattering (IXS) measurements of the dynamic structure factor in liquid Na57K43, sensitive to the atomic-scale coarse graining, reveal a sound velocity value exceeding the long wavelength, continuum value and indicate the coexistence of two phonon-like modes. Applying Generalized Collective Mode (GCM) analysis scheme, we show that the positive dispersion of the sound velocity occurs in a wavelength region below the crossover from hydrodynamic to atom-type excitations and, therefore, it can not be explained as sound propagation over the light specie (Na) network. The present result experimentally proves the existence of positive dispersion in a binary mixture due to a relaxation process, as opposed to fast sound phenomena.Comment: 7 pages, 8 figures, to appear in "Physical Review B

Single and Paired Point Defects in a 2D Wigner Crystal

Using the path-integral Monte Carlo method, we calculate the energy to form single and pair vacancies and interstitials in a two-dimensional Wigner crystal of electrons. We confirm that the lowest-lying energy defects of a 2D electron Wigner crystal are interstitials, with a creation energy roughly 2/3 that of a vacancy. The formation energy of the defects goes to zero near melting, suggesting that point defects might mediate the melting process. In addition, we find that the interaction between defects is strongly attractive, so that most defects will exist as bound pairs.Comment: 4 pages, 5 encapsulated figure

Role of Anisotropy and Refractive Index in Scattering and Whiteness Optimization

This is the final version. Available from Wiley via the DOI in this record.The ability to manipulate light–matter interaction to tailor the scattering properties of materials is crucial to many aspects of everyday life, from paints to lighting, and to many fundamental concepts in disordered photonics. Light transport and scattering in a granular disordered medium are dictated by the spatial distribution (structure factor) and the scattering properties (form factor and refractive index) of its building blocks. As yet, however, the importance of anisotropy in such systems has not been considered. Here, a systematic numerical survey that disentangles and quantifies the role of different kinds and degrees of anisotropy in scattering optimization is reported. It is shown that ensembles of uncorrelated, anisotropic particles with nematic ordering enables to increase by 20% the reflectance of low-refractive index media (n = 1.55), using only three-quarters of material compared to their isotropic counterpart. Additionally, these systems exhibit a whiteness comparable to conventionally used high-refractive index media, e.g., TiO2 (n = 2.60). Therefore, the findings not only provide an understanding of the role of anisotropy in scattering optimization, but they also showcase a novel strategy to replace inorganic white enhancers with sustainable and biocompatible products made of biopolymers.Biotechnology and Biological Sciences Research Council (BBSRC)European Research Council (ERC)Leverhulme Trus

Lattice-switch Monte Carlo

We present a Monte Carlo method for the direct evaluation of the difference between the free energies of two crystal structures. The method is built on a lattice-switch transformation that maps a configuration of one structure onto a candidate configuration of the other by `switching' one set of lattice vectors for the other, while keeping the displacements with respect to the lattice sites constant. The sampling of the displacement configurations is biased, multicanonically, to favor paths leading to `gateway' arrangements for which the Monte Carlo switch to the candidate configuration will be accepted. The configurations of both structures can then be efficiently sampled in a single process, and the difference between their free energies evaluated from their measured probabilities. We explore and exploit the method in the context of extensive studies of systems of hard spheres. We show that the efficiency of the method is controlled by the extent to which the switch conserves correlated microstructure. We also show how, microscopically, the procedure works: the system finds gateway arrangements which fulfill the sampling bias intelligently. We establish, with high precision, the differences between the free energies of the two close packed structures (fcc and hcp) in both the constant density and the constant pressure ensembles.Comment: 34 pages, 9 figures, RevTeX. To appear in Phys. Rev.

Geometrical Models of the Phase Space Structures Governing Reaction Dynamics

Hamiltonian dynamical systems possessing equilibria of ${saddle} \times {centre} \times...\times {centre}$ stability type display \emph{reaction-type dynamics} for energies close to the energy of such equilibria; entrance and exit from certain regions of the phase space is only possible via narrow \emph{bottlenecks} created by the influence of the equilibrium points. In this paper we provide a thorough pedagogical description of the phase space structures that are responsible for controlling transport in these problems. Of central importance is the existence of a \emph{Normally Hyperbolic Invariant Manifold (NHIM)}, whose \emph{stable and unstable manifolds} have sufficient dimensionality to act as separatrices, partitioning energy surfaces into regions of qualitatively distinct behavior. This NHIM forms the natural (dynamical) equator of a (spherical) \emph{dividing surface} which locally divides an energy surface into two components (`reactants' and `products'), one on either side of the bottleneck. This dividing surface has all the desired properties sought for in \emph{transition state theory} where reaction rates are computed from the flux through a dividing surface. In fact, the dividing surface that we construct is crossed exactly once by reactive trajectories, and not crossed by nonreactive trajectories, and related to these properties, minimizes the flux upon variation of the dividing surface. We discuss three presentations of the energy surface and the phase space structures contained in it for 2-degree-of-freedom (DoF) systems in the threedimensional space $\R^3$, and two schematic models which capture many of the essential features of the dynamics for $n$-DoF systems. In addition, we elucidate the structure of the NHIM.Comment: 44 pages, 38 figures, PDFLaTe

Metastable lifetimes in a kinetic Ising model: Dependence on field and system size

The lifetimes of metastable states in kinetic Ising ferromagnets are studied by droplet theory and Monte Carlo simulation, in order to determine their dependences on applied field and system size. For a wide range of fields, the dominant field dependence is universal for local dynamics and has the form of an exponential in the inverse field, modified by universal and nonuniversal power-law prefactors. Quantitative droplet-theory predictions are numerically verified, and small deviations are shown to depend nonuniversally on the details of the dynamics. We identify four distinct field intervals in which the field dependence and statistical properties of the lifetimes are different. The field marking the crossover between the weak-field regime, in which the decay is dominated by a single droplet, and the intermediate-field regime, in which it is dominated by a finite droplet density, vanishes logarithmically with system size. As a consequence the slow decay characteristic of the former regime may be observable in systems that are macroscopic as far as their equilibrium properties are concerned.Comment: 18 pages single spaced. RevTex Version 3. FSU-SCRI-94-1

Bio-inspired Highly Scattering Networks via Polymer Phase Separation

A common strategy to optimize whiteness in living organisms consists in using three-dimensional random networks with dense and polydisperse scattering elements constituted by relatively low-refractive index materials. Inspired by these natural architectures, we developed a fast and scalable method to produce highly scattering porous polymer films via phase separation. By varying the molecular weight of the polymer, we modified the morphology of the porous films and therefore tuned their scattering properties. The achieved transport mean free paths are in the micrometer range, improving the scattering strength of analogous low-refractive index systems, e.g. standard white paper, by an order of magnitude. The produced porous films show a broadband reflectivity of approximately 75 % whilst only 4 m thick. In addition, the films are flexible and can be readily index-matched with water (i.e. they become transparent when wet), allowing for various applications such as coatings with tunable transmittance and responsive paints

Dynamical properties of liquid Al near melting. An orbital-free molecular dynamics study

The static and dynamic structure of liquid Al is studied using the orbital free ab-initio molecular dynamics method. Two thermodynamic states along the coexistence line are considered, namely T = 943 K and 1323 K for which X-ray and neutron scattering data are available. A new kinetic energy functional, which fulfills a number of physically relevant conditions is employed, along with a local first principles pseudopotential. In addition to a comparison with experiment, we also compare our ab-initio results with those obtained from conventional molecular dynamics simulations using effective interionic pair potentials derived from second order pseudopotential perturbation theory.Comment: 15 pages, 12 figures, 2 tables, submitted to PR