Construction of an autonomous supramolecular system involved with hierarchy and its nonlinear dynamics.

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The catalyst ruthenium (II) tris-(2,2'-bipyridine)(Ru(bpy)_3) for Belousov-Zhabotinsky (BZ) reaction was covalently bonded to poly (N-isopropyl acrylamide) (PNIPA). When the poly(PNIPA+-co-Ru(bpy)_3) chain was dissolved into the BZ solution, the periodical coil-globule oscillation occurred. For the purpose to construct a hierarchical structure, we have tried to form microparticles based on poly(PNIPA+-co-Ru(bpy)3) in the BZ solution by the irradiation of an IR laser beam. Then we have observed the autonomous volume oscillation of the, microparticle (diameter【approximately equal】5μm) formed. Furthermore, we have prepared the water-in-oil microemulsion consisting of AOT, octane, and BZ reaction solution as active elements involved an autonomous function. We have provided the difference between the diffusion constant of the activator and that of the inhibitor by controlling external parameters, such as temperature, ionic strength, and volume fraction of droplets. As a result, we have foun … More d various reaction patterns such as the cluster wave and the non-annihilation wave.We have investigated the effect of hierarchization on self-organization through the stochastic resonance in the supramolecular system consisting of many excitable elements. We have used a one-dimensional array of excitable elements in which Belousov-Zhabotinsky (BZ) reaction was localized. We have found that (1) the degree of coherence of noise-induced oscillation is increased with increasing the number of elements, (2) phase locking between largely separated elements not interacting directly with each other is achieved via irregular oscillations of elements interposed between them, and (3) phase locking in a one-dimensional array of excitable elements is induced via coherence resonance of the first element. For a numerical simulation we have approximated the present system as a one-dimensional system consisting of four interacting excitable elements separated by an inactive area, i.e., a diffusion area. Experimental observations have been approximately reproduced in the numerical simulation with the three-variable Oregonator reaction-diffusion model modified to take into account the effects of an external electric noise. Less