期刊
JOURNAL OF CHEMICAL PHYSICS
卷 145, 期 21, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.4962216
关键词
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资金
- EPSRC [EP/E501311/1, EP/H00341X/1, EP/K000128/1]
- EPSRC [EP/K000233/1, EP/K000128/1, EP/H00341X/1, EP/G054940/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [1091213, EP/G054940/1, EP/K000233/1, EP/H00341X/1, EP/K000128/1] Funding Source: researchfish
We study a three-species analogue of the Potts lattice gas model of nucleation from solution in a regime where partially disordered solute is a viable thermodynamic phase. Using a multicanonical sampling protocol, we compute phase diagrams for the system, from which we determine a parameter regime where the partially disordered phase is metastable almost everywhere in the temperature-fugacity plane. The resulting model shows non-trivial nucleation and growth behaviour, which we examine via multidimensional free energy calculations. We consider the applicability of the model in capturing the multi-stage nucleation mechanisms of polymorphic biominerals (e.g., CaCO3). We then quantitatively explore the kinetics of nucleation in our model using the increasingly popular seeding method. We compare the resulting free energy barrier heights to those obtained via explicit free energy calculations over a wide range of temperatures and fugacities, carefully considering the propagation of statistical error. We find that the ability of the seeding method to reproduce accurate free energy barriers is dependent on the degree of supersaturation, and severely limited by the use of a nucleation driving force Delta mu computed for bulk phases. We discuss possible reasons for this in terms of underlying kinetic assumptions, and those of classical nucleation theory. (C) 2016 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).
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