Zimmermann, Nils. E. R., Vorselaars, Bart, Espinosa, Jorge R. , Quigley, David, Smith, William R., Sanz, Eduardo, Vega, Carlos and Peters, Baron (2018) NaCl nucleation from brine in seeded simulations: Sources of uncertainty in rate estimates. The Journal of Chemical Physics, 148 (22). p. 222838. ISSN 0021-9606
Full content URL: http://doi.org/10.1063/1.5024009
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Item Type: | Article |
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Item Status: | Live Archive |
Abstract
This work reexamines seeded simulation results for NaCl nucleation from a supersaturated aqueous solution at 298.15 K and 1 bar pressure. We present a linear regression approach for analyzing seeded simulation data that provides both nucleation rates and uncertainty estimates. Our results show that rates obtained from seeded simulations rely critically on a precise driving force for the model system. The driving force vs. solute concentration curve need not exactly reproduce that of the real system, but it should accurately describe the thermodynamic properties of the model system. We also show that rate estimates depend strongly on the nucleus size metric. We show that the rate estimates systematically increase as more stringent local order parameters are used to count members of a cluster and provide tentative suggestions for appropriate clustering criteria.
Keywords: | Crystallography, Brines, Electrolytes, Molecular dynamics, linear regression, adsorption, Computer simulation, thermodynamic properties |
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Subjects: | F Physical Sciences > F310 Applied Physics F Physical Sciences > F300 Physics F Physical Sciences > F200 Materials Science F Physical Sciences > F170 Physical Chemistry F Physical Sciences > F343 Computational Physics |
Divisions: | College of Science > School of Mathematics and Physics |
ID Code: | 32236 |
Deposited On: | 27 Jun 2018 20:44 |
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