Quantifying the Relevance of Long-Range Forces for Crystal Nucleation in Water

Zhao, Renjie; Zou, Ziyue; Weeks, John D.; Tiwary, Pratyush

doi:10.1021/acs.jctc.3c01120

Cited by 2 publications

(1 citation statement)

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“…It describes nucleation as a competition between the free energy cost for forming a surface (scaling as r 2 ) and the free energy benefit from a new crystalline phase (scaling as r 3 ) . CNT is an oversimplified model and completely overlooks the “two-step” mechanism in addition to other assumptions, often leading to significant errors in the nucleation rate even for simple systems. , As a result, it is not surprising that CNT is not able to describe the nucleation of other molecules with more complicated interactions or shapes, such as urea and glycine. , …”

Section: Introductionmentioning

confidence: 99%

Is the Local Ion Density Sufficient to Drive NaCl Nucleation from the Melt and Aqueous Solution?

Wang,

Mehdi,

Zou

et al. 2024

J. Phys. Chem. B

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Even though nucleation is ubiquitous in different science and engineering problems, investigating nucleation is extremely difficult due to the complicated ranges of time and length scales involved. In this work, we simulate NaCl nucleation in both molten and aqueous environments using enhanced sampling of all-atom molecular dynamics with deep-learning-based estimation of reaction coordinates. By incorporating various structural order parameters and learning the reaction coordinate as a function thereof, we achieve significantly improved sampling relative to traditional ad hoc descriptions of what drives nucleation, particularly in an aqueous medium. Our results reveal a one-step nucleation mechanism in both environments, with reaction coordinate analysis highlighting the importance of local ion density in distinguishing solid and liquid states. However, although fluctuations in the local ion density are necessary to drive nucleation, they are not sufficient. Our analysis shows that near the transition states, descriptors such as enthalpy and local structure become crucial. Our protocol proposed here enables robust nucleation analysis and phase sampling and could offer insights into nucleation mechanisms for generic small molecules in different environments.

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