Discrete aqueous solvent effects and possible attractive forces

We study discrete solvent effects on the interaction of two parallel charged surfaces in ionic aqueous solution. These effects are taken into account by adding a bilinear non-local term to the free energy of Poisson-Boltzmann theory. We study numerically the density profile of ions between the two plates, and the resulting inter-plate pressure. At large plate separations the two plates are decoupled and the ion distribution can be characterized by an effective Poisson-Boltzmann charge that is smaller than the nominal charge. The pressure is thus reduced relative to Poisson-Boltzmann predictions. At plate separations below ~2 nm the pressure is modified considerably, due to the solvent mediated short-range attraction between ions in the the system. For high surface charges this contribution can overcome the mean-field repulsion giving rise to a net attraction between the plates.Comment: 12 figures in 16 files. 19 pages. Submitted to J. Chem. Phys., July 200

Improved real-space genetic algorithm for crystal structure and polymorph prediction

Existing genetic algorithms for crystal structure and polymorph prediction can suffer from stagnation during evolution, with a consequent loss of efficiency and accuracy. An improved genetic algorithm is introduced herein which penalizes similar structures and so enhances structural diversity in the population at each generation. This is shown to improve the quality of results found for the theoretical prediction of simple model crystal structures. In particular, this method is demonstrated to find three new zero-temperature phases of the Dzugutov potential that have not been previously reported

Patterning of dielectric nanoparticles using dielectrophoretic forces generated by ferroelectric polydomain films

A theoretical study of a dielectrophoretic force, i.e. the force acting on an electrically neutral particle in the inhomogeneous electric field, which is produced by a ferroelectric domain pattern, is presented. It has been shown by several researchers that artificially prepared domain patterns with given geometry in ferroelectric single crystals represent an easy and flexible method for patterning dielectric nanoobjects using dielectrophoretic forces. The source of the dielectrophoretic force is a strong and highly inhomogeneous (stray) electric field, which exists in the vicinity of the ferroelectric domain walls at the surface of the ferroelectric film. We analyzed dielectrophoretic forces in the model of a ferroelectric film of a given thickness with a lamellar 180${}^\circ$ domain pattern. The analytical formula for the spatial distribution of the stray field in the ionic liquid above the top surface of the film is calculated including the effect of free charge screening. The spatial distribution of the dielectrophoretic force produced by the domain pattern is presented. The numerical simulations indicate that the intersection of the ferroelectric domain wall and the surface of the ferroelectric film represents a trap for dielectric nanoparticles in the case of so called positive dielectrophoresis. The effects of electrical neutrality of dielectric nanoparticles, free charge screening due to the ionic nature of the liquid, domain pattern geometry, and the Brownian motion on the mechanism of nanoparticle deposition and the stability of the deposited pattern are discussed.Comment: Accepted in the Journal of Applied Physics, 10 pages, 5 figure

Nonlinear dielectric effect of dipolar fluids

The nonlinear dielectric effect for dipolar fluids is studied within the framework of the mean spherical approximation (MSA) of hard core dipolar Yukawa fluids. Based on earlier results for the electric field dependence of the polarization our analytical results show so-called normal saturation effects which are in good agreement with corresponding NVT ensemble Monte Carlo simulation data. The linear and the nonlinear dielectric permittivities obtained from MC simulations are determined from the fluctuations of the total dipole moment of the system in the absence of an applied electric field. We compare the MSA based theoretical results with the corresponding Langevin and Debye-Weiss behaviors.Comment: 10 pages including 4 figure

All-Electron Path Integral Monte Carlo Simulations of Warm Dense Matter: Application to Water and Carbon Plasmas

We develop an all-electron path integral Monte Carlo (PIMC) method with free-particle nodes for warm dense matter and apply it to water and carbon plasmas. We thereby extend PIMC studies beyond hydrogen and helium to elements with core electrons. PIMC pressures, internal energies, and pair-correlation functions compare well with density functional theory molecular dynamics (DFT-MD) at temperatures of (2.5-7.5)$\times10^5$ K and both methods together form a coherent equation of state (EOS) over a density-temperature range of 3--12 g/cm$^3$ and 10$^4$--10$^9$ K

New Method to Calculate Electrical Forces Acting on a Sphere in an Electrorheological Fluid

We describe a method to calculate the electrical force acting on a sphere in a suspension of dielectric spheres in a host with a different dielectric constant, under the assumption that a spatially uniform electric field is applied. The method uses a spectral representation for the total electrostatic energy of the composite. The force is expressed as a certain gradient of this energy, which can be expressed in a closed analytic form rather than evaluated as a numerical derivative. The method is applicable even when both the spheres and the host have frequency-dependent dielectric functions and nonzero conductivities, provided the system is in the quasistatic regime. In principle, it includes all multipolar contributions to the force, and it can be used to calculate multi-body as well as pairwise forces. We also present several numerical examples, including host fluids with finite conductivities. The force between spheres approaches the dipole-dipole limit, as expected, at large separations, but departs drastically from that limit when the spheres are nearly in contact. The force may also change sign as a function of frequency when the host is a slightly conducting fluid.Comment: 29 pages, 8 figures, Accepted for Publication in Physical Review

Non-linear charge reduction effect in strongly-coupled plasmas

The charge reduction effect, produced by the nonlinear Debye screening of high-Z charges occuring in strongly-coupled plasmas, is investigated. An analytic asymptotic expression is obtained for the charge reduction factor which determines the Debye-Hueckel potential generated by a charged test particle. Its relevant parametric dependencies are analyzed and shown to predict a strong charge reduction effect in strongly-coupled plasmas.Comment: 4 figure

Comparison of methods for estimating continuous distributions of relaxation times

The nonparametric estimation of the distribution of relaxation times approach is not as frequently used in the analysis of dispersed response of dielectric or conductive materials as are other immittance data analysis methods based on parametric curve fitting techniques. Nevertheless, such distributions can yield important information about the physical processes present in measured material. In this letter, we apply two quite different numerical inversion methods to estimate the distribution of relaxation times for glassy \lila\ dielectric frequency-response data at 225 \kelvin. Both methods yield unique distributions that agree very closely with the actual exact one accurately calculated from the corrected bulk-dispersion Kohlrausch model established independently by means of parametric data fit using the corrected modulus formalism method. The obtained distributions are also greatly superior to those estimated using approximate functions equations given in the literature.Comment: 4 pages and 4 figure

Nonlinear screening of charged macromolecules

We present several aspects of the screening of charged macromolecules in an electrolyte. After a review of the basic mean field approach, based on the linear Debye-Huckel theory, we consider the case of highly charged macromolecules, where the linear approximation breaks down and the system is described by full nonlinear Poisson-Boltzmann equation. Some analytical results for this nonlinear equation give some interesting insight on physical phenomena like the charge renormalization and the Manning counterion condensation

Fractional Equations of Curie-von Schweidler and Gauss Laws

The dielectric susceptibility of most materials follows a fractional power-law frequency dependence that is called the "universal" response. We prove that in the time domain this dependence gives differential equations with derivatives and integrals of noninteger order. We obtain equations that describe "universal" Curie-von Schweidler and Gauss laws for such dielectric materials. These laws are presented by fractional differential equations such that the electromagnetic fields in the materials demonstrate "universal" fractional damping. The suggested fractional equations are common (universal) to a wide class of materials, regardless of the type of physical structure, chemical composition or of the nature of the polarization.Comment: 11 pages, LaTe