Designed patterns: flexible control of precipitation through electric currents.

Understanding and controlling precipitation patterns formed in reaction-diffusion processes is of fundamental importance with high potential for technical applications. Here we present a theory showing that precipitation resulting from reactions among charged agents can be controlled by an appropriately designed, time-dependent electric current. Examples of current dynamics yielding periodic bands of prescribed wavelength, as well as more complicated structures are given. The pattern control is demonstrated experimentally using the reaction-diffusion process 2AgNO3 + K2Cr2O7-->under Ag2Cr2O7 + 2KNO3.

Guiding fields for phase separation: controlling Liesegang patterns.

Liesegang patterns emerge from precipitation processes and may be used to build bulk structures at submicrometer length scales. Thus they have significant potential for technological applications provided adequate methods of control can be devised. Here we describe a simple, physically realizable pattern control based on the notion of driven precipitation, meaning that the phase separation is governed by a guiding field such as, for example, a temperature or pH field. The phase separation is modeled through a nonautonomous Cahn-Hilliard equation whose spinodal is determined by the evolving guiding field. Control over the dynamics of the spinodal gives control over the velocity of the instability front that separates the stable and unstable regions of the system. Since the wavelength of the pattern is largely determined by this velocity, the distance between successive precipitation bands becomes controllable. We demonstrate the above ideas by numerical studies of a one-dimensional system with a diffusive guiding field. We find that the results can be accurately described by employing a linear stability analysis (pulled-front theory) for determining the velocity-local-wavelength relationship. From the perspective of the Liesegang theory, our results indicate that the so-called revert patterns may be naturally generated by diffusive guiding fields.

Formation of Liesegang patterns in the presence of an electric field.

The effects of an external electric field on the formation of Liesegang patterns are investigated. The patterns are assumed to emerge from a phase separation process in the wake of a diffusive reaction front. The dynamics is described by a Cahn-Hilliard equation with a moving source term representing the reaction zone, and the electric field enters through its effects on the properties of the reaction zone. We employ our previous results [I. Bena, F. Coppex, M. Droz, and Z. Rácz, J. Chem. Phys. 122, 024512 (2005)] on how the electric field changes both the motion of the front, as well as the amount of reaction product left behind the front, and our main conclusion is that the number of precipitation bands becomes finite in a finite electric field. The reason for the finiteness in case when the electric field drives the reagents towards the reaction zone is that the width of consecutive bands increases so that, beyond a distance l(+), the precipitation is continuous (plug is formed). In case of an electric field of opposite polarity, the bands emerge in a finite interval l(-), since the reaction product decreases with time and the conditions for phase separation cease to exist. We give estimates of l(+/-) in terms of measurable quantities and thus present an experimentally verifiable prediction of the "Cahn-Hilliard equation with a moving source" description of Liesegang phenomena.

Front motion in an A+B-->C type reaction-diffusion process: effects of an electric field.

We study the effects of an external electric field on both the motion of the reaction zone and the spatial distribution of the reaction product, C, in an irreversible A- + B+ -->C reaction-diffusion process. The electrolytes A identical with (A+,A-) and B identical with (B+,B-) are initially separated in space and the ion-dynamics is described by reaction-diffusion equations obeying local electroneutrality. Without an electric field, the reaction zone moves diffusively leaving behind a constant concentration of C's. In the presence of an electric field which drives the reagents towards the reaction zone, we find that the reaction zone still moves diffusively but with a diffusion coefficient which slightly decreases with increasing field. The important electric field effect is that the concentration of C's is no longer constant but increases linearly in the direction of the motion of the front. The case of an electric field of reversed polarity is also discussed and it is found that the motion of the front has a diffusive as well as a drift component. The concentration of C's decreases in the direction of the motion of the front, up to the complete extinction of the reaction. Possible application of the above results to the understanding of the formation of Liesegang patterns in an electric field is briefly outlined.

Drift by dichotomous Markov noise.

We derive explicit results for the asymptotic probability density and drift velocity in systems driven by dichotomous Markov noise, including the situation in which the asymptotic dynamics crosses unstable fixed points. The results are illustrated on the problem of the rocking ratchet.

Yang-Lee zeros for an urn model for the separation of sand.

We apply the Yang-Lee theory of phase transitions to an urn model for the separation of sand. The effective partition function of this nonequilibrium system can be expressed as a polynomial of the size-dependent effective fugacity z. Numerical calculations show that in the thermodynamic limit the zeros of the effective partition function are located on the unit circle in the complex z plane. In the complex plane of the actual control parameter, certain roots converge to the transition point of the model. Thus, the Yang-Lee theory can be applied to a wider class of nonequilibrium systems than those considered previously.

Confinement of discrete breathers in inhomogeneously profiled nonlinear chains.

We investigate numerically the scattering of a moving discrete breather on a pair of junctions in a Fermi-Pasta-Ulam chain. These junctions delimit an extended region with different masses of the particles. We consider (i) a rectangular trap, (ii) a wedge shaped trap, and (iii) a smoothly varying convex or concave mass profile. All three cases lead to DB confinement, with the ease of trapping depending on the profile of the trap. We also study the collision and trapping of two DBs within the profile as a function of trap width, shape, and approach time at the two junctions. The latter controls whether one or both DBs are trapped.

Nonlinear response with dichotomous noise.

Dichotomous noise appears in a wide variety of physical and mathematical models. It has escaped attention that the standard results for the long time properties cannot be applied when unstable fixed points are crossed in the asymptotic regime. We show how calculations have to be modified to deal with these cases and present as a first application full analytic results for hypersensitive transport.

Velocity correlations, diffusion, and stochasticity in a one-dimensional system.

We consider the motion of a test particle in a one-dimensional system of equal-mass point particles. The test particle plays the role of a microscopic "piston" that separates two hard-point gases with different concentrations and arbitrary initial velocity distributions. In the homogeneous case when the gases on either side of the piston are in the same macroscopic state, we compute and analyze the stationary velocity autocorrelation function C(t). Explicit expressions are obtained for certain typical velocity distributions, serving to elucidate in particular the asymptotic behavior of C(t). It is shown that the occurrence of a nonvanishing probability mass at zero velocity is necessary for the occurrence of a long-time tail in C(t). The conditions under which this is a t(-3) tail are determined. Turning to the inhomogeneous system with different macroscopic states on either side of the piston, we determine its effective diffusion coefficient from the asymptotic behavior of the variance of its position, as well as the leading behavior of the other moments about the mean. Finally, we present an interpretation of the effective noise arising from the dynamics of the two gases, and thence that of the stochastic process to which the position of any particle in the system reduces in the thermodynamic limit.

Collective behavior of parametric oscillators.

We revisit the mean-field model of globally and harmonically coupled parametric oscillators subject to periodic block pulses with initially random phases. The phase diagram of regions of collective parametric instability is presented, as is a detailed characterization of the motions underlying these instabilities. This presentation includes regimes not identified in earlier work [I. Bena and C. Van den Broeck, Europhys. Lett. 48, 498 (1999)]. In addition to the familiar parametric instability of individual oscillators, two kinds of collective instabilities are identified. In one the mean amplitude diverges monotonically while in the other the divergence is oscillatory. The frequencies of collective oscillatory instabilities in general bear no simple relation to the eigenfrequencies of the individual oscillators nor to the frequency of the external modulation. Numerical simulations show that systems with only nearest-neighbor coupling have collective instabilities similar to those of the mean-field model. Many of the mean-field results are already apparent in a simple dimer [M. Copelli and K. Lindenberg, Phys. Rev. E 63, 036605 (2001)].

Hydrodynamic fluctuations in the kolmogorov flow: nonlinear regime

In a previous paper [I. Bena, M. Malek Mansour, and F. Baras, Phys. Rev. E 59, 5503 (1999)] the statistical properties of linearized Kolmogorov flow were studied, using the formalism of fluctuating hydrodynamics. In this paper the nonlinear regime is considered, with emphasis on the statistical properties of the flow near the first instability. The normal form amplitude equation is derived for the case of an incompressible fluid and the velocity field is constructed explicitly above (but close to) the instability. The relative simplicity of this flow allows one to analyze the compressible case as well. Using a perturbative technique, it is shown that close to the instability threshold the stochastic dynamics of the system is governed by two coupled nonlinear Langevin equations in Fourier space. The solution of these equations can be cast into the exponential of a Landau-Ginzburg functional, which proves to be identical to the one obtained for the case of an incompressible fluid. The theoretical predictions are confirmed by numerical simulations of the nonlinear fluctuating hydrodynamic equations.

Hydrodynamic fluctuations in the Kolmogorov flow: linear regime.

The Landau-Lifshitz fluctuating hydrodynamics is used to study the statistical properties of the linearized Kolmogorov flow. The relative simplicity of this flow allows a detailed analysis of the fluctuation spectrum from near equilibrium regime up to the vicinity of the first convective instability threshold. It is shown that in the long time limit the flow behaves as an incompressible fluid, regardless of the value of the Reynolds number. This is not the case for the short time behavior where the incompressibility assumption leads in general to a wrong form of the static correlation functions, except near the instability threshold. The theoretical predictions are confirmed by numerical simulations of the full nonlinear fluctuating hydrodynamic equations.