Forward flux sampling calculation of homogeneous nucleation rates from aqueous NaCl solutions

Jiang, Hao; Haji-Akbari, Amir; Debenedetti, Pablo G.; Panagiotopoulos, Athanassios Z.

doi:10.1063/1.5016554

Title: Forward flux sampling calculation of homogeneous nucleation rates from aqueous NaCl solutions

Journal Article · 24 January 2018 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/1.5016554 · OSTI ID:1512939

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Princeton Univ., NJ (United States). Dept. of Chemical and Biological Engineering; none
Yale Univ., New Haven, CT (United States). Dept. of Chemical and Environmental Engineering
Princeton Univ., NJ (United States). Dept. of Chemical and Biological Engineering

We used molecular dynamics simulations and the path sampling technique known as forward flux sampling to study homogeneous nucleation of NaCl crystals from supersaturated aqueous solutions at 298 K and 1 bar. Nucleation rates were obtained for a range of salt concentrations for the Joung-Cheatham NaCl force field combined with the Extended Simple Point Charge (SPC/E) water model. The calculated nucleation rates are significantly lower than the available experimental measurements. The estimates for the nucleation rates in this work do not rely on classical nucleation theory, but the pathways observed in the simulations suggest that the nucleation process is better described by classical nucleation theory than an alternative interpretation based on Ostwald’s step rule, in contrast to some prior simulations of related models. In addition to the size of NaCl nucleus, we find that the crystallinity of a nascent cluster plays an important role in the nucleation process. Nuclei with high crystallinity were found to have higher growth probability and longer lifetimes, possibly because they are less exposed to hydration water.

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Research Organization:: Princeton Univ., NJ (United States)

Sponsoring Organization:: USDOE; National Science Foundation (NSF)

Grant/Contract Number:: SC0002128

OSTI ID:: 1512939

Alternate ID(s):: OSTI ID: 1418078

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 4 Vol. 148; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Seeding approach to bubble nucleation in superheated Lennard-Jones fluids Rosales-Pelaez, P.; Garcia-Cid, M. I.; Valeriani, C. Physical Review E, Vol. 100, Issue 5 https://doi.org/10.1103/physreve.100.052609	journal	November 2019
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Nucleation in aqueous NaCl solutions shifts from 1-step to 2-step mechanism on crossing the spinodal Jiang, Hao; Debenedetti, Pablo G.; Panagiotopoulos, Athanassios Z. The Journal of Chemical Physics, Vol. 150, Issue 12 https://doi.org/10.1063/1.5084248	journal	March 2019
Calculation of critical nucleation rates by the persistent embryo method: application to quasi hard sphere models Ren, Shang; Sun, Yang; Zhang, Feng Soft Matter, Vol. 14, Issue 45 https://doi.org/10.1039/c8sm01415a	journal	January 2018
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