Journal of Chemical Physics, Vol.105, No.24, 10830-10837, 1996
Transitions in 2-Dimensional Patterns in a Ferrocyanide-Iodate-Sulfite Reaction
Transitions in two-dimensional (2D) spatial patterns were investigated in a ferrocyanide-iodate-sulfite (FIS) reaction in a circular thin,eel reactor. The state of the gel reactor was maintained by contact of one side of the gel with a continuously refreshed well-stirred reservoir. For long residence times of the chemicals in the reservoir, the gel reactor was in a spatially uniform state of low pH (about 4), while at short reservoir residence times the reactor was in a uniform state of high pH (about 7). At intermediate residence times the spatiotemporal 2D structures observed include a large low pH oscillating spot, small metastable high pH oscillating spots, shrinking rings, spirals that formed when the axisymmetry of shrinking rings was broken, self-replicating spots that either grew and divided or died from overcrowding, and highly irregular, stationary lamellae. Transitions among the different patterns were examined as a function of gel thickness (0.2-0.6 mm), reservoir residence time (0.6-4 min), and ferrocyanide concentration (12-80 mM). Iodate and sulfite concentrations were held fixed at 75.0 and 89.0 mM, respectively. Several transitions were examined in detail : from a stationary spot to an oscillating spat; from an oscillating spot to a shrinking ring or spirals; the onset of replicating spots; and the transition from a homogeneous state to lamellar patterns. The observed phenomena can all be described in terms of a parity-breaking front bifurcation (nonequilibrium Ising-Bloch bifurcation).