Short-time rotational diffusion in monodisperse charge-stabilized colloidal suspensions

We investigate the combined effects of electrostatic interactions and hydrodynamic interactions on the short-time rotational self-diffusion coefficient in charge-stabilized suspensions. We calculate this coefficient as a function of volume fraction for various effective particle charges and amounts of added electrolyte. The influence of the hydrodynamic interactions on the rotational diffusion coefficient is less pronounced for charged particles than for uncharged ones. Salt-free suspensions are weakly influenced by hydrodynamic interactions. For these strongly correlated systems we obtain a quadratic volume fraction-dependence of the diffusion coefficient, which is well explained in terms of an effective hard sphere model.Comment: 21 pages, LaTeX, 7 Postscript figures included using epsf, to appear in Physica

Non-monotonic density dependence of the diffusion of DNA fragments in low-salt suspensions

The high linear charge density of 20-base-pair oligomers of DNA is shown to lead to a striking non-monotonic dependence of the long-time self-diffusion on the concentration of the DNA in low-salt conditions. This generic non-monotonic behavior results from both the strong coupling between the electrostatic and solvent-mediated hydrodynamic interactions, and from the renormalization of these electrostatic interactions at large separations, and specifically from the dominance of the far-field hydrodynamic interactions caused by the strong repulsion between the DNA fragments.Comment: 4 pages, 2 figures. Physical Review E, accepted on November 24, 200

Electrokinetic and hydrodynamic properties of charged-particles systems: From small electrolyte ions to large colloids

Dynamic processes in dispersions of charged spherical particles are of importance both in fundamental science, and in technical and bio-medical applications. There exists a large variety of charged-particles systems, ranging from nanometer-sized electrolyte ions to micron-sized charge-stabilized colloids. We review recent advances in theoretical methods for the calculation of linear transport coefficients in concentrated particulate systems, with the focus on hydrodynamic interactions and electrokinetic effects. Considered transport properties are the dispersion viscosity, self- and collective diffusion coefficients, sedimentation coefficients, and electrophoretic mobilities and conductivities of ionic particle species in an external electric field. Advances by our group are also discussed, including a novel mode-coupling-theory method for conduction-diffusion and viscoelastic properties of strong electrolyte solutions. Furthermore, results are presented for dispersions of solvent-permeable particles, and particles with non-zero hydrodynamic surface slip. The concentration-dependent swelling of ionic microgels is discussed, as well as a far-reaching dynamic scaling behavior relating colloidal long- to short-time dynamics

Enhanced structural correlations accelerate diffusion in charge-stabilized colloidal suspensions

Theoretical calculations for colloidal charge-stabilized and hard sphere suspensions show that hydrodynamic interactions yield a qualitatively different particle concentration dependence of the short-time self-diffusion coefficient. The effect, however, is numerically small and hardly accessible by conventional light scattering experiments. Applying multiple-scattering decorrelation equipment and a careful data analysis we show that the theoretical prediction for charged particles is in agreement with our experimental results from aqueous polystyrene latex suspensions.Comment: 1 ps-file (MS-Word), 14 page

Self-diffusion coefficients of charged particles: Prediction of Nonlinear volume fraction dependence

We report on calculations of the translational and rotational short-time self-diffusion coefficients $D^t_s$ and $D^r_s$ for suspensions of charge-stabilized colloidal spheres. These diffusion coefficients are affected by electrostatic forces and many-body hydrodynamic interactions (HI). Our computations account for both two-body and three-body HI. For strongly charged particles, we predict interesting nonlinear scaling relations $D^t_s\propto 1-a_t\phi^{4/3}$ and $D^r_s\propto 1-a_r\phi^2$ depending on volume fraction $\phi$, with essentially charge-independent parameters $a_t$ and $a_r$. These scaling relations are strikingly different from the corresponding results for hard spheres. Our numerical results can be explained using a model of effective hard spheres. Moreover, we perceptibly improve the known result for $D^t_s$ of hard sphere suspensions.Comment: 8 pages, LaTeX, 3 Postscript figures included using eps

Assessment of electrophoresis and electroosmosis in construction materials: effect of enhancing electrolytes and heavy metals contamination

Electrokinetic effects are those that take place by application of an electric field to porous materials, with the zeta potential as the key parameter. Specifically, in the case of contaminated construction materials, the generation of an electroosmotic flux, with the corresponding dragging due to water transport, is a crucial mechanism to succeed in the treatment of decontamination. Therefore, it is of great interest trying to optimize the treatment by the addition of specific electrolytes enhancing the electrokinetic phenomena. Most of the data of zeta potential found in literature for construction materials are based in micro-electrophoresis measurements, which are quite far of the real conditions of application of the remediation treatments. In this paper, electrophoretic and electroosmotic experiments, with monolithic and powdered material respectively, have been carried out for mortar, brick and granite clean and contaminated with Cs, Sr, Co, Cd, Cu and Pb. The electrolytes tested have been distilled water (DW), Na2–EDTA, oxalic acid, acetic acid and citric acid. The zeta potential values have been determined through the two different techniques and the results compared and critically analysed

A simple patchy colloid model for the phase behavior of lysozyme dispersions

We propose a minimal model for spherical proteins with aeolotopic pair interactions to describe the equilibrium phase behavior of lysozyme. The repulsive screened Coulomb interactions between the particles are taken into account assuming that the net charges are smeared out homogeneously over the spherical protein surfaces. We incorporate attractive surface patches, with the interactions between patches on different spheres modeled by an attractive Yukawa potential. The parameters entering the attractive Yukawa potential part are determined using information on the experimentally accessed gas-liquid-like critical point. The Helmholtz free energy of the fluid and solid phases is calculated using second-order thermodynamic perturbation theory. Our predictions for the solubility curve are in fair agreement with experimental data. In addition, we present new experimental data for the gas-liquid coexistence curves at various salt concentrations and compare these with our model calculations. In agreement with earlier findings, we observe that the strength and the range of the attractive potential part only weakly depend on the salt content

Decoherence times of universal two-qubit gates in the presence of broad-band noise

The controlled generation of entangled states of two quantum bits is a fundamental step toward the implementation of a quantum information processor. In nano-devices this operation is counteracted by the solid-state environment, characterized by a broadband and non-monotonic power spectrum, often 1/f at low frequencies. For single-qubit gates, incoherent processes due to fluctuations acting on different time scales result in peculiar short- and long-time behavior. Markovian noise gives rise to exponential decay with relaxation and decoherence times, T1 and T2, simply related to the symmetry of the qubit-environment coupling Hamiltonian. Noise with the 1/f power spectrum at low frequencies is instead responsible for defocusing processes and algebraic short-time behavior. In this paper, we identify the relevant decoherence times of an entangling operation due to the different decoherence channels originating from solid-state noise. Entanglement is quantified by concurrence, which we evaluate in an analytic form employing a multi-stage approach. The 'optimal' operating conditions of reduced sensitivity to noise sources are identified. We apply this analysis to a superconducting \sqrt{i-SWAP} gate for experimental noise spectra.Comment: 35 pages, 11 figure

A corresponding states approach to Small-Angle-Scattering for polydisperse ionic colloidal fluids

Approximate scattering functions for polydisperse ionic colloidal fluids are obtained by a corresponding states approach. This assumes that all pair correlation functions $g_{\alpha \beta}(r)$ of a polydisperse fluid are conformal to those of an appropriate monodisperse binary fluid (reference system) and can be generated from them by scaling transformations. The correspondence law extends to ionic fluids a {\it scaling approximation} (SA) successfully proposed for nonionic colloids in a recent paper. For the primitive model of charged hard spheres in a continuum solvent, the partial structure factors of the monodisperse binary reference system are evaluated by solving the Orstein-Zernike (OZ) integral equations coupled with an approximate closure. The SA is first tested within the mean spherical approximation (MSA) closure, which allows analytical solutions. The results are found in good overall agreement with exact MSA predictions up to relevant polidispersity. The SA is shown to be an improvement over the ``decoupling approximation'' extended to the ionic case. The simplicity of the SA scheme allows its application also when the OZ equations can be solved only numerically. An example is then given by using the hypernetted chain (HNC) closure. Shortcomings of the SA approach, its possible use in the analysis of experimental scattering data and other related points are also briefly addressed.Comment: 29 pages, 7 postscript figures (included), Latex 3.0, uses aps.sty, to appear in Phys. Rev. E (1999

Gaussian density fluctuations, mode coupling theory, and all that

We consider a toy model for glassy dynamics of colloidal suspensions: a single Brownian particle diffusing among immobile obstacles. If Gaussian factorization of static density fluctuations is assumed, this model can be solved without factorization approximation for any dynamic correlation function. The solution differs from that obtained from the ideal mode coupling theory (MCT). The latter is equivalent to including only some, positive definite terms in an expression for the memory function. An approximate re-summation of the complete expression suggests that, under the assumption of Gaussian factorization of static fluctuations, mobile particle's motion is always diffusive. In contrast, MCT predicts that the mobile particle becomes localized at a high enough obstacle density. We discuss the implications of these results for models for glassy dynamics.Comment: to be published in Europhys. Let