Effect of substrate mismatch, orientation, and flexibility on heterogeneous ice nucleation

Abstract

Heterogeneous nucleation is the main path to ice formation on Earth. The ice nucleating ability of a certain substrate is mainly determined by both molecular interactions and the structural mismatch between the ice and the substrate lattices. We focus on the latter factor using molecular simulations of the mW model. Quantifying the effect of structural mismatch alone is challenging due to its coupling with molecular interactions. To disentangle both factors, we use a substrate composed of water molecules in such a way that any variation on the nucleation temperature can be exclusively ascribed to the structural mismatch. We find that a one per cent increase of structural mismatch leads to a decrease of approximately 4 K in the nucleation temperature. We also analyse the effect of the orientation of the substrate with respect to the liquid. The three main ice orientations (basal, primary prism and secondary prism) have a similar ice nucleating ability. We finally asses the effect of lattice flexibility by comparing substrates where molecules are immobile with others where a certain freedom to fluctuate around the lattice positions is allowed. Interestingly, we find that the latter type of substrate is more efficient in nucleating ice because it can adapt its structure to that of ice.

Energy units in Fig. 3 is "kcal/mol", not "kJ/mol"

References in corpus (11)

• The Many Faces of Heterogeneous Ice Nucleation: Interplay Between Surface Morphology and Hydrophobicity
• Molecular simulations of heterogeneous ice nucleation. I. Controlling ice nucleation through surface hydrophilicity
• Ice Nucleation on Carbon Surface Supports the Classical Theory for Heterogeneous Nucleation
• Ice Formation on Kaolinite: Insights from Molecular Dynamics Simulations
• The Microscopic Features of Heterogeneous Ice Nucleation May Affect the Macroscopic Morphology of Atmospheric Ice Crystals
• Interfacial Free Energy as the Key to the Pressure-Induced Deceleration of Ice Nucleation
• Heterogeneous ice nucleation on silver-iodide-like surfaces
• Molecular simulations of heterogeneous ice nucleation. II. Peeling back the layers
• Absence of superheating for ice Ih with a free surface : a new method of determining the melting point of different water models
• Effects of surface interactions on heterogeneous ice nucleation for a monatomic water model
• Homogeneous Ice Nucleation Rate in Water Droplets

Cited by in corpus (1)

• Heterogeneous ice nucleation on model substrates