Premelting layer during ice growth: role of clusters

Abstract

The premelting layer plays an important role in ice growth, but there is a significant gap in our knowledge between the atomistic premelting surface structure and the macroscopic growth mechanism. In this work, using large-scale molecular dynamics simulation, we reveal the existence of clusters on the premelting surface, as an intermediate feature bridging the gap. We show the spontaneous formation and evolution of clusters, and they form a stable distribution determined by the growth rate. We demonstrate how this stable distribution is related to the growth mode of ice, connected by the growth of clusters. We come to a bilayer-by-bilayer growth mode at simulation-reachable high growth rates, but another mechanism, namely "cluster stacking", is speculated to exist at lower growth rates. This work builds a connection between the microscopic structure of the premelting layer and the macroscopic growth of ice, making a step forward toward the full understanding of premelting and ice growth.