Abstract
The theory of homogeneous nucleation is developed for a model nonlinear bistable chemical reaction driven far from equilibrium (trimolecular Schlögl model). The theory is restricted to the vicinity of the stable/unstable transition, where the nucleation barrier is small but nonvanishing. The nucleation rates are derived for two types of fluctuations: first, fluctuations due to a homogeneous external white noise source, and second, internal chemical fluctuations, described by a reastion-diffusion multivariate master equation. In the white noise case, a Landau-Ginzburg potential can be defined, and the standard nucleation formalism can be applied; this is not true for the internal case and a new result is used. The inhomogeneous chemical fluctuations, due to the coupling between the nonlinear reaction and diffusion, are shown to have an influence on the nucleation rate. Quantitative conditions are also given to evaluate the possibility of homogeneous nucleation in nonlinear chemical systems.
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Borgis, D., Moreau, M. Nucleation theory for a model bistable chemical reaction. J Stat Phys 50, 935–962 (1988). https://doi.org/10.1007/BF01019148
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DOI: https://doi.org/10.1007/BF01019148