Microscopic Mechanism and Kinetics of Ice Formation at Complex Interfaces: Zooming in on Kaolinite

Abstract

Most ice in nature forms thanks to impurities which boost the exceedingly low nucleation rate of pure supercooled water. However, the microscopic details of ice nucleation on these substances remain largely unknown. Here, we have unraveled the molecular mechanism and the kinetics of ice formation on kaolinite, a clay mineral playing a key role in climate science. We find that the formation of ice at strong supercooling in the presence of this clay is twenty orders of magnitude faster than homogeneous freezing. The critical nucleus is substantially smaller than that found for homogeneous nucleation and, in contrast to the predictions of classical nucleation theory (CNT), it has a strong 2D character. Nonetheless, we show that CNT describes correctly the formation of ice at this complex interface. Kaolinite also promotes the exclusive nucleation of hexagonal ice, as opposed to homogeneous freezing where a mixture of cubic and hexagonal polytypes is observed.

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Cited by in corpus (8)

• Ice Formation on Kaolinite: Insights from Molecular Dynamics Simulations
• Nucleation in aqueous NaCl solutions shifts from 1-step to 2-step mechanism on crossing the spinodal
• Studying Rare Events using Forward-Flux Sampling: Recent Breakthroughs and Future Outlook
• What Makes a Good Descriptor for Heterogeneous Ice Nucleation on OH-Patterned Surfaces
• Contour forward flux sampling: Sampling rare events along multiple collective variables
• Can molecular simulations reliably compare homogeneous and heterogeneous ice nucleation?
• The Impact of Hydration Shell Inclusion and Chain Exclusion in the Efficacy of Reaction Coordinates for Homogeneous and Heterogeneous Ice Nucleation
• Memory Control of Ice Growth During Non-Equilibrium Freezing of Water