Elucidating the mechanism of nucleation near the gas-liquid spinodal

Bhimalapuram, Prabhakar ; Chakrabarty, Suman ; Bagchi, Biman (2007) Elucidating the mechanism of nucleation near the gas-liquid spinodal Physical Review Letters, 98 (20). 206104_1-206104_4. ISSN 0031-9007

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Official URL: http://prl.aps.org/abstract/PRL/v98/i20/e206104

Related URL: http://dx.doi.org/10.1103/PhysRevLett.98.206104


We have constructed a multidimensional free energy surface of nucleation of the liquid phase from the parent supercooled and supersaturated vapor phase near the gas-liquid spinodal. In particular, we remove the Becker-Doring constraint of having only one growing cluster in the system. Close to the spinodal, the free energy, as a function of the size of the largest cluster, develops surprisingly a minimum at a subcritical cluster size. It is this minimum at intermediate size that is found to be responsible for the barrier towards further growth of the nucleus at large supersaturation. An alternative free energy pathway involving the participation of many subcritical clusters is found near the spinodal where the growth of the nucleus is promoted by a coalescence mechanism. The growth of the stable phase becomes collective and spatially diffuse, and the significance of a 'critical nucleus' is lost for deeper quenches.

Item Type:Article
Source:Copyright of this article belongs to American Physical Society.
Keywords:Nucleation; Growth; Spinodal Decomposition; Classical Nucleation Theory; non-Boltzmann Sampling
ID Code:3979
Deposited On:13 Oct 2010 07:07
Last Modified:16 May 2016 14:39

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