Effects of lateral diffusion on morphology and dynamics of a microscopic lattice-gas model of pulsed electrodeposition

Abstract

The influence of nearest-neighbor diffusion on the decay of a metastable low-coverage phase (monolayer adsorption) in a square lattice-gas model of electrochemical metal deposition is investigated by kinetic Monte Carlo simulations. The phase-transformation dynamics are compared to the well-established Kolmogorov-Johnson-Mehl-Avrami theory. The phase transformation is accelerated by diffusion, but remains in accord with the theory for continuous nucleation up to moderate diffusion rates. At very high diffusion rates the phase-transformation kinetic shows a crossover to instantaneous nucleation. Then, the probability of medium-sized clusters is reduced in favor of large clusters. Upon reversal of the supersaturation, the adsorbate desorbs, but large clusters still tend to grow during the initial stages of desorption. Calculation of the free energy of subcritical clusters by enumeration of lattice animals yields a quasi-equilibrium distribution which is in reasonable agreement with the simulation results. This is an improvement relative to classical droplet theory, which fails to describe the distributions, since the macroscopic surface tension is a bad approximation for small clusters.

Minor corrections and modifications. 15 pages with 10 figures. Accepted for publication in the Journal of Chemical Physics, see http://jcp.aip.org/jcp/

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• Kinetic Monte Carlo simulations of electrodeposition: Crossover from continuous to instantaneous homogeneous nucleation within Avrami's law
• Response of a Model of CO Oxidation with CO Desorption and Diffusion to a Periodic External CO Pressure
• Driven-dissipative ising model: mean field solution
• New Cyclic Voltammetry Method for Examining Phase Transitions: Simulated Results
• Dynamics of Desorption with Lateral Diffusion