Lifanov, Yuri, Vorselaars, Bart and Quigley, David (2016) Nucleation barrier reconstruction via the seeding method in a lattice model with competing nucleation pathways. The Journal of Chemical Physics, 145 (21). pp. 1-12. 211912. doi:10.1063/1.4962216

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Abstract

We study a three-species analogue of the Potts Lattice Gas (PLG) model of nucleation from solution in a regime where partially disordered solute is a viable thermodynamic phase. Using a muilticanonical 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 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 ∆μ computed for bulk phases. We discuss possible reasons for this in terms of underlying kinetic assumptions, and those of classical nucleation theory.

Item Type:	Journal Article
Subjects:	Q Science > QD Chemistry
Divisions:	Faculty of Science > Centre for Complexity Science Faculty of Science > Physics Faculty of Science > Centre for Scientific Computing
Library of Congress Subject Headings (LCSH):	Nucleation, Lattice theory
Journal or Publication Title:	The Journal of Chemical Physics
Publisher:	American Institute of Physics
ISSN:	0021-9606
Official Date:	13 September 2016
Dates:	Date Event 13 September 2016 Available 22 August 2016 Accepted 8 June 2016 Submitted
Date of first compliant deposit:	15 September 2016
Volume:	145
Number:	21
Number of Pages:	12
Page Range:	pp. 1-12
Article Number:	211912
DOI:	10.1063/1.4962216
Status:	Peer Reviewed
Publication Status:	Published
Access rights to Published version:	Open Access
RIOXX Funder/Project Grant:	Project/Grant ID RIOXX Funder Name Funder ID EP/E501311/1 [EPSRC] Engineering and Physical Sciences Research Council http://dx.doi.org/10.13039/501100000266 EP/H00341X/1 [EPSRC] Engineering and Physical Sciences Research Council http://dx.doi.org/10.13039/501100000266 EP/K000128/1 [EPSRC] Engineering and Physical Sciences Research Council http://dx.doi.org/10.13039/501100000266
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