NaCl nucleation from brine in seeded simulations: Sources of uncertainty in rate estimates

Zimmermann, Nils. E.  R.; Vorselaars, Bart; Espinosa, Jorge R.; Quigley, David; Smith, William R.; Sanz, Eduardo; Vega, Carlos; Peters, Baron

doi:10.1063/1.5024009

Title: NaCl nucleation from brine in seeded simulations: Sources of uncertainty in rate estimates

Journal Article · 29 May 2018 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/1.5024009 · OSTI ID:1506316

^[1];

^[2]; Espinosa, Jorge R. ^[3];

^[4];

^[5]; Sanz, Eduardo ^[3];

^[3]; Peters, Baron ^[6]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of Lincoln (United Kingdom)
Universidad Complutense de Madrid (Spain)
Univ. of Warwick (United Kingdom)
Univ. of Guelph, ON (Canada)
Univ. of California, Santa Barbara, CA (United States)

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.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Materials Sciences & Engineering Division (SC- 22.2)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1506316

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 22 Vol. 148; ISSN 0021-9606

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

Country of Publication:: United States

Language:: English

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