Physics – Condensed Matter – Materials Science
Scientific paper
2004-09-20
J. Chem. Phys. 122, 064705 (2005)
Physics
Condensed Matter
Materials Science
Minor corrections and modifications. 15 pages with 10 figures. Accepted for publication in the Journal of Chemical Physics, se
Scientific paper
10.1063/1.1847653
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.
Frank Stefan
Rikvold Per Arne
Roberts Daniel E.
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