Spatial bistability: a source of complex dynamics. From spatiotemporal reaction-diffusion patterns to chemomechanical structures

We show experimentally and theoretically that reaction systems characterized by a slow induction period followed by a fast evolution to equilibrium can readily generate "spatial bistability" when operated in thin gel reactors diffusively fed from one side. This phenomenon which corresponds to the coexistence of two different stable steady states, not breaking the symmetry of the boundary conditions, can be at the origin of diverse reaction-diffusion instabilities. Using different chemical reactions, we show how stationary pulses, labyrinthine patterns or spatiotemporal oscillations can be generated. Beyond simple reaction-diffusion instabilities, we also demonstrate that the cross coupling of spatial bistability with the size responsiveness of a chemosensitive gel can give rise to autonomous spatiotemporal shape patterns, referred to as chemomechanical structures.     

Chemical turbulence and standing waves in a surface reaction model: The influence of global coupling and wave instabilities

Among heterogeneously catalyzed chemical reactions, the CO oxidation on the Pt(110) surface under vacuum conditions offers probably the greatest wealth of spontaneous formation of spatial patterns. Spirals, fronts, and solitary pulses were detected at low surface temperatures (T<500 K), in line with the standard phenomenology of bistable, excitable, and oscillatory reaction-diffusion systems. At high temperatures (T greater, similar 540 K), more surprising features like chemical turbulence and standing waves appeared in the experiments. Herein, we study a realistic reaction-diffusion model of this system, with respect to the latter phenomena. In particular, we deal both with the influence of global coupling through the gas phase on the oscillatory reaction and the possibility of wave instabilities under excitable conditions. Gas-phase coupling is shown to either synchronize the oscillations or to yield turbulence and standing structures. The latter findings are closely related to clustering in networks of coupled oscillators and indicate a dominance of the global gas-phase coupling over local coupling via surface diffusion. In the excitable regime wave instabilities in one and two dimensions have been discovered. In one dimension, pulses become unstable due to a vanishing of the refractory zone. In two dimensions, turbulence can also emerge due to spiral breakup, which results from a violation of the dispersion relation.     

Pattern formation in the ferrocyanide-iodate-sulfite reaction: the control of space scale separation

We revisit the conditions for the development of reaction-diffusion patterns in the ferrocyanide-iodate-sulfite bistable and oscillatory reaction. This hydrogen ion autoactivated reaction is the only example known to produce sustained stationary lamellar patterns and a wealth of other spatio-temporal phenomena including self-replication and localized oscillatory domain of spots, due to repulsive front interactions and to a parity-breaking front bifurcation (nonequilibrium Ising-Bloch bifurcation). We show experimentally that the space scale separation necessary for the observation of stationary patterns is mediated by the presence of low mobility weak acid functional groups. The presence of such groups was overlooked in the original observations made with hydrolyzable polyacrylamide gels. This missing information made the original observations difficult to reproduce and frustrated further experimental exploitation of the fantastic potentialities of this system. Using one-side-fed spatial reactors filled with agarose gel, we can reproduce all the previous pattern observations, in particular the stationary labyrinthine patterns, by introducing, above a critical concentration, well controlled amounts of polyacrylate chains in the gel network. We use two different geometries of spatial reactors (annular and disk shapes) to provide complementary information on the actual three-dimensional character of spatial patterns. We also reinvestigate the role of other feed parameters and show that the system exhibits both a domain of spatial bistability and of large-amplitude pH oscillations associated in a typical cross-shape diagram. The experimental method presented here can be adapted to produce patterns in the large number of oscillatory and bistable reactions, since the iodate-sulfite-ferrocynide reaction is a prototype of these systems.     

Pattern formation in the thiourea-iodate-sulfite system: Spatial bistability, waves, and stationary patterns

We present a detailed study of the reaction-diffusion patterns observed in the thiourea-iodate-sulfite (TuIS) reaction, operated in open one-side-fed reactors. Besides spatial bistability and spatio-temporal oscillatory dynamics, this proton autoactivated reaction shows stationary patterns, as a result of two back-to-back Turing bifurcations, in the presence of a low-mobility proton binding agent (sodium polyacrylate). This is the third aqueous solution system to produce stationary patterns and the second to do this through a Turing bifurcation. The stationary pattern forming capacities of the reaction are explored through a systematic design method, which is applicable to other bistable and oscillatory reactions. The spatio-temporal dynamics of this reaction is compared with that of the previous ferrocyanide-iodate-sulfite mixed Landolt system.     

Limit cycles of the ballast resistor caused by intrinsic instabilities

Spatio-temporal patterns of the ballast resistor are investigated. It is well known that in a voltage-controlled ballast resistor an electrothermal instability leads to stable stationary states consisting of hot and cold domains. Such states may become oscillatory unstable, giving rise to the bifurcation of limit cycles. These limit cycles are not caused by the external circuit but by a recently proposed novel intrinsic mechanism. There are two types of oscillatory instabilities: bulk instabilities and boundary-induced instabilities. The bulk instabilities are caused by resistivities which are not monotonically increasing functions of the temperature. The boundary-induced instabilities occur in small systems with Neumann boundary conditions. To find the bulk instability, experiments with materials showing a metal-semiconductor transition or high-temperature superconductors are suggested. To understand these new phenomena, the equation of motion is reduced to ordinary differential equations where the instabilities can be discussed analytically.     

Singular Limit of a Reaction-Diffusion Equation with a Spatially Inhomogeneous Reaction Term

We study reaction-diffusion equations with a spatially inhomogeneous reaction term. If the coefficient of these reaction term is much larger than the diffusion coefficient, a sharp interface appears between two different phases. We show that the equation of motion of such an interface involves a drift term despite the absence of drift in the original diffusion equations. In particular, we show that the same rich spatial patterns observed for a chemotaxis-growth model can be realized by a system without a drift term.     

Quasisoliton interaction of pursuit-evasion waves in a predator-prey system

We consider a system of partial differential equations describing two spatially distributed populations in a "predator-prey" interaction with each other. The spatial evolution is governed by three processes: positive taxis of predators up the gradient of prey (pursuit), negative taxis of prey down the gradient of predators (evasion), and diffusion resulting from random motion of both species. We demonstrate a new type of propagating wave in this system. The mechanism of propagation of these waves essentially depends on the taxis and is entirely different from waves in a reaction-diffusion system. Unlike typical reaction-diffusion waves, which annihilate on collision, these "taxis" waves can often penetrate through each other and reflect from impermeable boundaries.     

Wave grouping of a meandering spiral induced by Doppler effects and oscillatory dispersion

A new type of meandering spiral pattern, in which the dense waves form groups while the sparse waves keep evenly spaced, is observed in a spatial open reactor using a ferroin-catalyzed Belousov-Zhabotinsky reaction. Such a phenomenon is related to both the Doppler effect of a meandering spiral and the oscillatory dispersion relation of the system. Simulation in the two-dimensional Oregonator reaction-diffusion model with an oscillatory dispersion relation gives very similar results.     

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.     

反应扩散系统中时空斑图研究

时空斑图广泛地存在于反应扩散系统中,在延展的布鲁塞尔振子模型中,一维的时空斑图已经被研究过.本文中,我们对布鲁塞尔振子模型进行线性稳定性分析,模拟出两维的时空斑图,进一步阐明斑图形成的机制,形成斑图的机制是由于霍普夫失稳、短波失稳和图灵失稳以及它们之间的相互作用.当系统处于非平衡状态下,布鲁塞尔振子模型可以得到有序的时空斑图.?     

Front reversals, wave traps, and twisted spirals in periodically forced oscillatory media

A new kind of nonlinear nonequilibrium patterns--twisted spiral waves--is predicted for periodically forced oscillatory reaction-diffusion media. We show, furthermore, that, in such media, spatial regions with modified local properties may act as traps where propagating waves can be stored and released in a controlled way. Underlying both phenomena is the effect of the wavelength-dependent propagation reversal of traveling phase fronts, always possible when homogeneous oscillations are modulationally stable without forcing. The analysis is performed using as a model the complex Ginzburg-Landau equation, applicable for reaction-diffusion systems in the vicinity of a supercritical Hopf bifurcation.     

Local excitation-lateral inhibition interaction yields oscillatory instabilities in nonlocally interacting systems involving finite propagation delay

The work studies wave activity in spatial systems, which exhibit nonlocal spatial interactions at the presence of a finite propagation speed. We find analytically propagation delay-induced oscillatory instabilities for various local excitatory and lateral inhibitory spatial interactions. Further, the work shows for general nonlocal interactions analytically that the first kernel Fourier moment defines the stability thresholds. The final numerical simulation confirms the analytical results.     

Nonsteady waves in distributed dynamical systems

The paper is devoted to the study of one-dimensional and two-dimensional transient wave regimes in nonlinear systems of the reaction-diffusion type. In a one-dimensional case the process of collision of two travelling waves is considered. It is demonstrated that in the case of a nondispersive nonlinear system, where a steady regime of the collision is not possible, the process can be described by means of an approximation which is nonuniform in a spatial coordinate. The collision results, in a general case, in formation of an oscillatory shock wave moving with varying velocity. In a two-dimensional situation the transition of a rotating vortex into a rotating spiral wave in the case of dispersive systems and the inverse transition in the case of nondispersive systems are considered.     

Resonantly forced inhomogeneous reaction-diffusion systems

The dynamics of spatiotemporal patterns in oscillatory reaction-diffusion systems subject to periodic forcing with a spatially random forcing amplitude field are investigated. Quenched disorder is studied using the resonantly forced complex Ginzburg-Landau equation in the 3:1 resonance regime. Front roughening and spontaneous nucleation of target patterns are observed and characterized. Time dependent spatially varying forcing fields are studied in the 3:1 forced FitzHugh-Nagumo system. The periodic variation of the spatially random forcing amplitude breaks the symmetry among the three quasi-homogeneous states of the system, making the three types of fronts separating phases inequivalent. The resulting inequality in the front velocities leads to the formation of "compound fronts" with velocities lying between those of the individual component fronts, and "pulses" which are analogous structures arising from the combination of three fronts. Spiral wave dynamics is studied in systems with compound fronts. (c) 2000 American Institute of Physics.     

Rhombic patterns: Broken hexagonal symmetry

Landau-Ginzburg equations derived to conserve two-dimensional spatial symmetries lead to the prediction that rhombic arrays with characteristic angles slightly differ from 60 degrees should form in many systems. Beyond the bifurcation from the uniform state to patterns, rhombic patterns are linearly stable for a band of angles near the 60 degrees angle of regular hexagons. Experiments conducted on a reaction-diffusion system involving a chlorite-iodide-malonic acid reaction yield rhombic patterns in good accord with the theory.     

反应扩散系统中螺旋波的失稳

文章以反应扩散系统为例,介绍了在可激发系统与振荡系统中螺旋波产生、发展、演化的一些基本性质及规律,并讨论了作者近年来对螺旋波的各种失稳途径、时空混沌的产生机理及螺旋波控制方面所做的实验与理论工作,重点讨论了两类螺旋波失稳现象：爱克豪斯失稳与多普勒失稳,两类失稳都使系统从有规律的螺旋波态变为时空混沌（缺陷湍流）态。     

Entropy-driven phase transitions with influence of the field-dependent diffusion coefficient

We present a comprehensive study of phase transitions in a single-field reaction-diffusion stochastic systems with a field-dependent mobility of a power-law form and internal fluctuations. Using variational principles and mean-field theory we have shown that the noise can sustain spatial patterns and leads to phase transitions type of “order-disorder”. These phase transitions can be critical and non-critical in character. Our theoretical results are verified by computer simulations.     

Self-sustained spatiotemporal oscillations induced by membrane-bulk coupling

We propose a novel mechanism leading to spatiotemporal oscillations in extended systems that does not rely on local bulk instabilities. Instead, oscillations arise from the interaction of two subsystems of different spatial dimensionality. Specifically, we show that coupling a passive diffusive bulk of dimension d with an excitable membrane of dimension d-1 produces a self-sustained oscillatory behavior. An analytical explanation of the phenomenon is provided for d=1. Moreover, in-phase and antiphase synchronization of oscillations are found numerically in one and two dimensions. This novel dynamic instability could be used by biological systems such as cells, where the dynamics on the cellular membrane is necessarily different from that of the cytoplasmic bulk.