INTERFACE PROPAGATION AND NUCLEATION PHENOMENA FOR DISCONTINUOUS POISONING TRANSITIONS IN SURFACE-REACTION MODELS

被引:53
作者
EVANS, JW [1 ]
RAY, TR [1 ]
机构
[1] IOWA STATE UNIV SCI & TECHNOL, DEPT MATH, AMES, IA 50011 USA
关键词
D O I
10.1103/PhysRevE.50.4302
中图分类号
O35 [流体力学]; O53 [等离子体物理学];
学科分类号
070204 ; 080103 ; 080704 ;
摘要
Here, we consider discontinuous nonequilibrium phase transitions to poisoned or adsorbing states in lattice-gas models of surface reactions. Specifically, we examine the monomer or CO-poisoning transition in the Ziff-Gulari-Barshad monomer-dimer reaction model for CO oxidation, modified to include adspecies diffusion. For CO pressures below the poisoning transition, we first characterize the propagation of and fluctuations at an interface between reactive and CO-poisoned states. Here, we utilize ideas from spatial contact models, reaction-diffusion theory, and kinetic roughening theory. Evolution is described by the Kardar-Parisi-Zhang equation, but with the nonlinearity and kinetic surface tension vanishing on approaching the transition. Next, again for CO pressures below the transition, we consider the evolution of a nucleus of the reactive state embedded in the CO-poisoned state, now exploiting concepts from epidemic theory. We elucidate the divergence and sharpening of the critical size of this nucleus, both approaching the transition and with increasing adspecies diffusion rates. The deviation from mean-field divergence approaching the transition is related to the vanishing of the kinetic surface tension. The sharpening is related to the reduced influence of fluctuations. Throughout this contribution, we focus on providing a unifying framework that can describe both the fluctuation-dominated behavior of the lattice-gas model for low adspecies diffusion rates, and the crossover to the deterministic mean-field behavior for high diffusion rates where the adlayer is well mixed or randomized. © 1994 The American Physical Society.
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页码:4302 / 4314
页数:13
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