Abstract
In this paper we discuss how the information contained in atomistic simulations of homogeneous nucleation should be used when fitting the parameters in macroscopic nucleation models. We show how the number of solid and liquid atoms in such simulations can be determined unambiguously by using a Gibbs dividing surface and how the free energy as a function of the number of solid atoms in the nucleus can thus be extracted. We then show that the parameters of a model based on classical nucleation theory can be fit using the information contained in these freeenergy profiles but that the parameters in such models are highly correlated. This correlation is unfortunate as it ensures that small errors in the computed free energy surface can give rise to large errors in the extrapolated properties of the fitted model. To resolve this problem we thus propose a method for fitting macroscopic nucleation models that uses simulations of planar interfaces and simulations of threedimensional nuclei in tandem. We show that when the parameters of the macroscopic model are fitted in this way the numerical errors for the final fitted model are smaller and that the extrapolated predictions for large nuclei are thus more reliable.
Original language  English 

Article number  104707 
Number of pages  6 
Journal  Journal of Chemical Physics 
Volume  14 
Issue number  10 
DOIs  
Publication status  Published  13 Sep 2017 
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Gareth Tribello
 School of Mathematics and Physics  Senior Lecturer
 Research Centre in Sustainable Energy
 Atomistic Simulation Centre (ASC)
Person: Academic