Stability of convective patterns in reaction fronts: a comparison of three models

Autocatalytic reaction fronts generate density gradients that may lead to convection. Fronts propagating in vertical tubes can be flat, axisymmetric, or nonaxisymmetric, depending on the diameter of the tube. In this paper, we study the transitions to convection as well as the stability of different types of fronts. We analyze the stability of the convective reaction fronts using three different models for front propagation. We use a model based on a reaction-diffusion-advection equation coupled to the Navier-Stokes equations to account for fluid flow. A second model replaces the reaction-diffusion equation with a thin front approximation where the front speed depends on the front curvature. We also introduce a new low-dimensional model based on a finite mode truncation. This model allows a complete analysis of all stable and unstable fronts.     

The effect of convection on a propagating front with a liquid product: Comparison of theory and experiments

This work is devoted to the investigation of propagating polymerization fronts converting a liquid monomer into a liquid polymer. We consider a simplified mathematical model which consists of the heat equation and equation for the depth of conversion for one-step chemical reaction and of the Navier-Stokes equations under the Boussinesq approximation. We fulfill the linear stability analysis of the stationary propagating front and find conditions of convective and thermal instabilities. We show that convection can occur not only for ascending fronts but also for descending fronts. Though in the latter case the exothermic chemical reaction heats the cold monomer from above, the instability appears and can be explained by the interaction of chemical reaction with hydrodynamics. Hydrodynamics changes also conditions of the thermal instability. The front propagating upwards becomes less stable than without convection, the front propagating downwards more stable. The theoretical results are compared with experiments. The experimentally measured stability boundary for polymerization of benzyl acrylate in dimethyl formamide is well approximated by the theoretical stability boundary. (c) 1998 American Institute of Physics.     

Poiseuille advection of chemical reaction fronts

Poiseuille flow between parallel plates alters the shapes and velocities of chemical reaction fronts. In the narrow-gap limit, the cubic reaction-diffusion-advection equation predicts a front-velocity correction equal to the gap-averaged fluid velocity epsilon. In the singular wide-gap limit, the correction equals the midgap fluid velocity 3epsilon/2 when the flow is in the direction of propagation of the reaction front, and equals zero for adverse flow of any amplitude for which the front has a midgap cusp. Stationary fronts are possible only for adverse flow and finite gaps. Experiments are suggested.     

The effects of fluid motion on oscillatory and chaotic fronts

We study oscillatory and chaotic reaction fronts described by the Kuramoto-Sivashinsky equation coupled to different types of fluid motion. We first apply a Poiseuille flow on the fronts inside a two-dimensional slab. We show regions of period doubling transition to chaos for different values of the average speed of Poiseuille flow. We also analyze the effects of a convective flow due to a Rayleigh-Taylor instability. Here the front is a thin interface separating two fluids of different densities inside a two-dimensional vertical slab. Convection is caused by buoyancy forces across the front as the lighter fluid is under a heavier fluid. We first obtain oscillatory and chaotic solutions arising from instabilities intrinsic to the front. Then, we determine the changes on the solutions due to fluid motion.     

A geometric approach to bistable front propagation in scalar reaction–diffusion equations with cut-off

‘Cut-offs’ were introduced to model front propagation in reaction–diffusion systems in which the reaction is effectively deactivated at points where the concentration lies below some threshold. In this article, we investigate the effects of a cut-off on fronts propagating into metastable states in a class of bistable scalar equations. We apply the method of geometric desingularization from dynamical systems theory to calculate explicitly the change in front propagation speed that is induced by the cut-off. We prove that the asymptotics of this correction scales with fractional powers of the cut-off parameter, and we identify the source of these exponents, thus explaining the structure of the resulting expansion. In particular, we show geometrically that the speed of bistable fronts increases in the presence of a cut-off, in agreement with results obtained previously via a variational principle. We first discuss the classical Nagumo equation as a prototypical example of bistable front propagation. Then, we present corresponding results for the (equivalent) cut-off Schlögl equation. Finally, we extend our analysis to a general family of reaction–diffusion equations that support bistable fronts, and we show that knowledge of an explicit front solution to the associated problem without cut-off is necessary for the correction induced by the cut-off to be computable in closed form.     

Convection in chemical fronts with quadratic and cubic autocatalysis

Convection in chemical fronts enhances the speed and determines the curvature of the front. Convection is due to density gradients across the front. Fronts propagating in narrow vertical tubes do not exhibit convection, while convection develops in tubes of larger diameter. The transition to convection is determined not only by the tube diameter, but also by the type of chemical reaction. We determine the transition to convection for chemical fronts with quadratic and cubic autocatalysis. We show that quadratic fronts are more stable to convection than cubic fronts. We compare these results to a thin front approximation based on an eikonal relation. In contrast to the thin front approximation, reaction-diffusion models show a transition to convection that depends on the ratio between the kinematic viscosity and the molecular diffusivity. (c) 2002 American Institute of Physics.     

Global Solutions to a Reactive Boussinesq System with Front Data on an Infinite Domain

We prove the existence of global solutions to a coupled system of Navier–Stokes, and reaction-diffusion equations (for temperature and mass fraction) with prescribed front data on an infinite vertical strip or tube. This system models a one-step exothermic chemical reaction. The heat release induced volume expansion is accounted for via the Boussinesq approximation. The solutions are time dependent moving fronts in the presence of fluid convection. In the general setting, the fronts are subject to intensive Rayleigh-Taylor and thermal-diffusive instabilities. Various physical quantities, such as fluid velocity, temperature, and front speed, can grow in time. We show that the growth is at most for large time t by constructing a nonlinear functional on the temperature and mass fraction components. These results hold for arbitrary order reactions in two space dimensions and for quadratic and cubic reactions in three space dimensions. In the absence of any thermal-diffusive instability (unit Lewis number), and with weak fluid coupling, we construct a class of fronts moving through shear flows. Although the front speeds may oscillate in time, we show that they are uniformly bounded for large t. The front equation shows the generic time-dependent nature of the front speeds and the straining effect of the flow field. Received: 15 January 1996 / Accepted: 2 September 1997     

Dynamics of one- and two-dimensional kinks in bistable reaction-diffusion equations with quasidiscrete sources of reaction

We study the evolution of fronts in a bistable reaction-diffusion system when the nonlinear reaction term is spatially inhomogeneous. This equation has been used to model wave propagation in various biological systems. Extending previous works on homogeneous reaction terms, we derive asymptotically an equation governing the front motion, which is strongly nonlinear and, for the two-dimensional case, generalizes the classical mean curvature flow equation. We study the motion of one- and two-dimensional fronts, finding that the inhomogeneity acts as a "potential function" for the motion of the front; i.e., there is wave propagation failure and the steady state solution depends on the structure of the function describing the inhomogeneity. (c) 2001 American Institute of Physics.     

Dynamics of A + B --> C reaction fronts in the presence of buoyancy-driven convection

The dynamics of A+B-->C fronts in horizontal solution layers can be influenced by buoyancy-driven convection as soon as the densities of A, B, and C are not all identical. Such convective motions can lead to front propagation even in the case of equal diffusion coefficients and initial concentration of reactants for which reaction-diffusion (RD) scalings predict a nonmoving front. We show theoretically that the dynamics in the presence of convection can in that case be predicted solely on the basis of the knowledge of the one-dimensional RD density profile across the front.     

Effect of interfacial tension on propagating polymerization fronts

This paper is devoted to the investigation of polymerization fronts converting a liquid monomer into a liquid polymer. We assume that the monomer and the polymer are immiscible and study the influence of the interfacial tension on the front stability. The mathematical model consists of the reaction-diffusion equations coupled with the Navier-Stokes equations through the convection terms. The jump conditions at the interface take into account the interfacial tension. Simple physical arguments show that the same temperature distribution could not lead to Marangoni instability for a nonreacting system. We fulfill a linear stability analysis and show that interaction of the chemical reaction and of the interfacial tension can lead to an instability that has another mechanism: the heat produced by the reaction decreases the interfacial tension and initiates the liquid motion. It brings more monomer to the reaction zone and increases even more the heat production. This feedback mechanism can lead to the instability if the frontal Marangoni number exceeds a critical value. (c) 2000 American Institute of Physics.     

Mapping the local reaction kinetics by PEEM: CO oxidation on individual (100)-type grains of Pt foil

The locally-resolved reaction kinetics of CO oxidation on individual (100)-type grains of a polycrystalline Pt foil was monitored in situ using photoemission electron microscopy (PEEM). Reaction-induced surface morphology changes were studied by optical differential interference contrast microscopy and atomic force microscopy (AFM). Regions of high catalytic activity, low activity and bistability in a (p,T)-parameter space were determined, allowing to establish a local kinetic phase diagram for CO oxidation on (100) facets of Pt foil. PEEM observations of the reaction front propagation on Pt(100) domains reveal a high degree of propagation anisotropy both for oxygen and CO fronts on the apparently isotropic Pt(100) surface. The anisotropy vanishes for oxygen fronts at temperatures above 465?K, but is maintained for CO fronts at all temperatures studied, i.e. in the range of 417 to 513?K. A change in the front propagation mechanism is proposed to explain the observed effects.     

Dynamics of interface in three-dimensional anisotropic bistable reaction-diffusion system

This paper presents a theoretical investigation of dynamics of interface (wave front) in three-dimensional (3D) reaction-diffusion (RD) system for bistable media with anisotropy constructed by means of anisotropic surface tension. An equation of motion for the wave front is derived to carry out stability analysis of transverse perturbations, which discloses mechanism of pattern formation such as labyrinthine in 3D bistable media. Particularly, the effects of anisotropy on wave propagation are studied. It was found that, sufficiently strong anisotropy can induce dynamical instabilities and lead to breakup of the wave front. With the fast-inhibitor limit, the bistable system can further be described by a variational dynamics so that the boundary integral method is adopted to study the dynamics of wave fronts.     

Front propagation into an unstable state of reaction-transport systems

We studied the propagation of traveling fronts into an unstable state of the reaction-transport systems involving integral transport. By using a hyperbolic scaling procedure and singular perturbation techniques, we determined a Hamiltonian structure of reaction-transport equations. This structure allowed us to derive asymptotic formulas for the propagation rate of a reaction front. We showed that the macroscopic dynamics of the front are "nonuniversal" and depend on the choice of the underlying random walk model for the microscopic transport process.     

Scaling,propagation, and kinetic roughening of flame fronts in random media

We introduce a model of two coupled reaction-diffusion equations to describe the dynamics and propagation of flame fronts in random media. The model incorporates heat diffusion, its dissipation, and its production through coupling to the background reactant density. We first show analytically and numerically that there is a finite critical value of the background density below which the front associated with the temperature field stops propagating. The critical exponents associated with this transition are shown to be consistent with meanfield theory of percolation. Second, we study the kinetic roughening associated with a moving planar flame front above the critical density. By numerically calculating the time-dependent width and equal-time height correlation function of the front, we demonstrate that the roughening process belongs to the universality class of the Kardar-Parisi-Zhang interface equation. Finally, we show how this interface equation can be analytically derived from our model in the limit of almost uniform background density.     

The propagation of discontinuities in non-homogeneous thermoviscoelastic media

In this study, the propagation of plane, cylindrical and spherical dilatational waves in non-homogeneous thermoviscoelastic media is investigated by employing the notion of singular surfaces and the method of characteristics. The inhomogeneity of the medium is such that the material properties depend in an arbitrary manner on the co-ordinate coinciding with the direction of the propagation. An integral type constitutive equation is considered for the heat flux which permits a finite propagation speed for thermal disturbances. It is found that the application of a dynamic input on the boundary surface gives rise to two different wave fronts along which mechanical and thermal effects are coupled. The growth and decay equations describing the change of the strength of the discontinuities on these two wave fronts are then obtained. By integrating the growth and decay equations along the rays the solutions valid at the wave fronts are found. The solutions are then reduced to two special cases: in one the heat flux equation is taken as the so-called modified Fourier equation, and in the other as the classical Fourier equation. The effects of inhomogeneity, geometry of the wave front, thermomechanical coupling and material internal friction on the strength of the discontinuity are discussed.     

Wave front fragmentation due to ventricular geometry in a model of the rabbit heart

The role of the heart's complex shape in causing the fragmentation of activation wave fronts characteristic of ventricular fibrillation (VF) has not been well studied. We used a finite element model of cardiac propagation capable of simulating functional reentry on curved two-dimensional surfaces to test the hypothesis that uneven surface curvature can cause local propagation block leading to proliferation of reentrant wave fronts. We found that when reentry was induced on a flat sheet, it rotated in a repeatable meander pattern without breaking up. However, when a model of the rabbit ventricles was formed from the same medium, reentrant wave fronts followed complex, nonrepeating trajectories. Local propagation block often occurred when wave fronts propagated across regions where the Gaussian curvature of the surface changed rapidly. This type of block did not occur every time wave fronts crossed such a region; rather, it only occurred when the wave front was very close behind the previous wave in the cycle and was therefore propagating into relatively inexcitable tissue. Close wave front spacing resulted from nonstationary reentrant propagation. Thus, uneven surface curvature and nonstationary reentrant propagation worked in concert to produce wave front fragmentation and complex activation patterns. None of the factors previously thought to be necessary for local propagation block (e.g., heterogeneous refractory period, steep action potential duration restitution) were present. We conclude that the complex geometry of the heart may be an important determinant of VF activation patterns. (c) 2002 American Institute of Physics.     

Determination of the Kardar–Parisi–Zhang equation from experimental data with a small number of configurations

We introduce an inverse method to determine the parameters of the Kardar–Parisi–Zhang equation corresponding to an evolving interface which requires a small number of configurations as input data. Our approach presents advantages for applications in real world scenarios since it does not require small time intervals between fronts. The method is applied to a restricted solid-on-solid model and a stochastic cellular automata model for fire front propagation.