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P De Kepper

Publications and source records attributed to P De Kepper.

7 recordsLinked to original sources

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.

Catalysis↗

Spatial bistability in a pH autocatalytic system: from long to short range activation.

The acid-auto-activated chlorite-tetrathionate reaction is studied in a one-side-fed spatial reactor. It was previously shown that in these conditions the unstirred reaction-diffusion system can generate oscillatory and excitable states even though under well-stirred nonequilibrium conditions only steady-state bistability is observed. Numerical simulations suggest that these temporal reaction-diffusion instabilities result from long-range activation by rapidly diffusing protons. We study here experimentally and numerically the effect of introducing into this reaction-diffusion system macromolecular carboxylate species that reduce the effective diffusivity of protons. Consistent with the original assumption, the introduction of such slow mobility proton-binding species quenches both oscillatory and excitability dynamics. Within the bistability domain the direction of the propagation of an interface between the two steady states depends on control parameter value. We elaborate on the fact that beyond a low critical concentration of macromolecular carboxylate species, the stability limit of the "thermodynamic" branch of spatial steady state does not depend on this concentration. Despite the relative simplicity of the kinetic model used in the numerical simulations, the results are in quasi-quantitative agreement with the experimental observations.

Journal Article↗

Destabilization of Turing structures by electric fields.

The dynamic behavior of hexagonal Turing patterns in the chlorine dioxide-iodine-malonic acid reaction was studied in a newly developed open reactor under the influence of externally applied weak directed current up to 17.5 mA. A transition from stationary hexagonal patterns to spots moving parallel to the direction of the applied electric field could be observed. The velocity of the drift increases monotonously with the applied current. Experimental results could be qualitatively reproduced in numerical simulations with a reaction-diffusion-advection model, based on a realistic kinetic mechanism.

Journal Article↗

Dynamical effects induced by long range activation in a nonequilibrium reaction-diffusion system.

We show both experimentally and numerically that the time scales separation introduced by long range activation can induce oscillations and excitability in nonequilibrium reaction-diffusion systems that would otherwise only exhibit bistability. Namely, we show that in the chlorite-tetrathionate reaction, where the autocatalytic species H+ diffuses faster than the substrates, the spatial bistability domain in the nonequilibrium phase diagram is extended with oscillatory and excitability domains. A simple model and a more realistic model qualitatively account for the observed dynamical behavior. The latter model provides quantitative agreement with the experiments.

Journal Article↗

Spatial bistability and waves in a reaction with acid autocatalysis.

The phenomenon of spatial bistability has recently been proposed for a comprehensive understanding of a number of chemical patterns observed in open spatial reactors consisting of thin films of gel diffusively fed from one side. We study experimentally and numerically this phenomenon in the tetrathionate-chlorite reaction characterized by an acid superautocatalysis. We focus on the similarities and differences with previous studies on the chlorine dioxide-iodide reaction. In addition, we show that this reaction, which is only bistable in a continuous stirred tank reactor, can exhibit oscillatory and traveling waves when diffusion comes into play. Our computations suggest that the nonstationary behaviour originates from differential diffusive transport.

Journal Article↗

Chemical morphogenesis: turing patterns in an experimental chemical system.

Patterns resulting from the sole interplay between reaction and diffusion are probably involved in certain stages of morphogenesis in biological systems, as initially proposed by Alan Turing. Self-organization phenomena of this type can only develop in nonlinear systems (i.e. involving positive and negative feedback loops) maintained far from equilibrium. We present Turing patterns experimentally observed in a chemical system. An oscillating chemical reaction, the CIMA reaction, is operated in an open spatial reactor designed in order to obtain a pure reaction-diffusion system. The two types of Turing patterns observed, hexagonal arrays of spots and parallel stripes, are characterized by an intrinsic wavelength. We identify the origin of the necessary diffusivity between activator and inhibitor. We also describe a pattern growth mechanism by spot splitting that recalls cell division.

Animals↗

Experimental study of synchronization phenomena under periodic light irradiation of a nonlinear chemical system.

A photosensitive chemical oscillating reaction, i.e., the Briggs-Rauscher (B.R.) reaction, exhibiting a wealth of nonlinear behavior, when performed in a continuous-flow stirred-tank reactor, and subjected to periodic light irradiation, is studied as an experimental example of entrainment phenomena observable in biological systems. The adaptation patterns under periodic light irradiation are elucidated by means of the response of the system to continuous and single-pulse light irradiation. It is shown that self-oscillating states, excitable steady states and bistable systems can exhibit the same types of synchronization patterns when submitted to periodic external forces with appropriate amplitude and time scale conditions.

Journal Article↗