9 research outputs found
Phase transitions and crossovers in reaction-diffusion models with catalyst deactivation
The activity of catalytic materials is reduced during operation by several
mechanisms, one of them being poisoning of catalytic sites by chemisorbed
impurities or products. Here we study the effects of poisoning in two
reaction-diffusion models in one-dimensional lattices with randomly distributed
catalytic sites. Unimolecular and bimolecular single-species reactions are
considered, without reactant input during the operation. The models show
transitions between a phase with continuous decay of reactant concentration and
a phase with asymptotic non-zero reactant concentration and complete poisoning
of the catalyst. The transition boundary depends on the initial reactant and
catalyst concentrations and on the poisoning probability. The critical system
behaves as in the two-species annihilation reaction, with reactant
concentration decaying as t^{-1/4} and the catalytic sites playing the role of
the second species. In the unimolecular reaction, a significant crossover to
the asymptotic scaling is observed even when one of those parameters is 10% far
from criticality. Consequently, an effective power-law decay of concentration
may persist up to long times and lead to an apparent change in the reaction
kinetics. In the bimolecular single-species reaction, the critical scaling is
followed by a two-dimensional rapid decay, thus two crossovers are found.Comment: 8 pages, 7 figure
Temperature Effects in the Initial Stages of Heteroepitaxial Film Growth
Kinetic Monte Carlo simulations of a model of thin film heteroepitaxy are performed to investigate the effects of the deposition temperature in the initial growth stages. Broad ranges of the rates of surface processes are used to model materials with several activation energies and several temperature changes, in conditions of larger diffusivity on the substrate in comparison with other film layers. When films with the same coverage are compared, the roughness increases with the deposition temperature in the regimes of island growth, coalescence, and initial formation of the continuous films. Concomitantly, the position of the minimum of the autocorrelation function is displaced to larger sizes. These apparently universal trends are consequences of the formation of wider and taller islands, and are observed with or without Ehrlich-Schwöebel barriers for adatom diffusion at step edges. The roughness increase with temperature qualitatively matches the observations of recent works on the deposition of inorganic and organic materials. In thicker films, simulations with some parameter sets show the decrease of roughness with temperature. In these cases, a re-entrance of roughness may be observed in the initial formation of the continuous films