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Journal Articles Journal of Physical Chemistry A Year : 2020

Microcanonical Nucleation Theory for Anisotropic Materials Validated on Alumina Clusters

Abstract

Nucleation kinetics in gas phase remains an open issue with no general model. The derivation of the reaction constants assuming a canonical ensemble fails to describe anisotropic materials such as oxides. We have developed a general and versatile model using activated complex kinetics with a microcanonical approach. This approach handles the kinetics issue in cluster growth when the transient nature of the processes hinders the use of the canonical ensemble. The model efficiently reproduces experimental size distributions of alumina clusters formed by laser ablation with different buffer gas densities, including magic numbers. We show that the thermodynamic equilibrium is not reached during the growth. The bounding energy measured is 10 times lower than the one deduced from DFT calculation, but also the one expected from the bulk cohesive energy.
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hal-03229945 , version 1 (19-05-2021)

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Arsène Chemin, Ken Miyajima, Patrice Melinon, Fumitaka Mafuné, David Amans. Microcanonical Nucleation Theory for Anisotropic Materials Validated on Alumina Clusters. Journal of Physical Chemistry A, 2020, 124 (11), pp.2328-2334. ⟨10.1021/acs.jpca.0c01038⟩. ⟨hal-03229945⟩
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