Understanding the sensitivity of nucleation free energies: The role of supersaturation and temperature

Samuel J. Keasler, J. Ilja Siepmann

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Abstract

Simulations are used to investigate the vapor-to-liquid nucleation of water for several different force fields at various sets of physical conditions. The nucleation free energy barrier is found to be extremely sensitive to the force field at the same absolute conditions. However, when the results are compared at the same supersaturation and reduced temperature or the same metastability parameter and reduced temperature, then the differences in the nucleation free energies of the different models are dramatically reduced. This finding suggests that comparisons of experimental data and computational predictions are most meaningful at the same relative conditions and emphasizes the importance of knowing the phase diagram of a given computational model, but such information is usually not available for models where the interaction energy is determined directly from electronic structure calculations.

Original languageEnglish (US)
Article number164516
JournalJournal of Chemical Physics
Volume143
Issue number16
DOIs
StatePublished - Jan 1 2015

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