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Kinetic theory of diffusion-limited nucleation
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Physical Metallurgy.
2016 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 144, no 20, 204501Article in journal (Refereed) PublishedText
Abstract [en]

We examine binary nucleation in the size and composition space {R, c} using the formalism of the multivariable theory [N. V. Alekseechkin, J. Chem. Phys. 124, 124512 (2006)]. We show that the variable c drops out of consideration for very large curvature of the new phase Gibbs energy with composition. Consequently nuclei around the critical size have the critical composition, which is derived from the condition of criticality for the canonical variables and is found not to depend on surface tension. In this case, nucleation kinetics can be investigated in the size space only. Using macroscopic kinetics, we determine the general expression for the condensation rate when growth is limited by bulk diffusion, which accounts for both diffusion and capillarity and exhibits a different dependence with the critical size, as compared with the interface-limited regime. This new expression of the condensation rate for bulk diffusion-limited nucleation is the counterpart of the classical interface-limited result. We then extend our analysis to multicomponent solutions.

Place, publisher, year, edition, pages
American Institute of Physics (AIP), 2016. Vol. 144, no 20, 204501
Keyword [en]
Condensation, Growth kinetics, Kinetics, Nucleation, Binary nucleation, Canonical variables, Condensation rates, Critical composition, General expression, Macroscopic kinetics, Multicomponent solutions, Nucleation kinetics
National Category
Physical Chemistry
URN: urn:nbn:se:kth:diva-189682DOI: 10.1063/1.4950878ISI: 000377712700040PubMedID: 27250310ScopusID: 2-s2.0-84971260942OAI: diva2:948326

QC 20160711

Available from: 2016-07-11 Created: 2016-07-11 Last updated: 2016-07-11Bibliographically approved

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Bonvalet, Manon
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