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Insights into the Emerging Networks of Voids in Simulated Supercooled Water.

The structural evolution of supercooled liquid water as we approach the glass transition temperature continues to be an active area of research. Here, we use molecular dynamics simulations of TIP4P/Ice to study the changes in the connected regions of empty space within the liquid which we interrogate using the Voronoi-voids network. We observe two important features: supercooling enhances the fraction of non-spherical voids and different sizes of voids tend to cluster forming a percolating network. By examining order parameters such as the local structure index (LSI), tetrahedrality and topological defects, we show that water molecules near large void clusters tend to be slightly more tetrahedral than those near small voids, with a lower population of under- and over-coordinated defects. We show further that the distribution of closed rings of water molecules around small and large void clusters maintain a balance between 6 and 7 membered rings. Our results highlight the changes of the dual voids and water network as a structural hallmark of supercooling which provides insights into the molecular origins of cooperative effects that underlie density fluctuations occurring on the sub-nanometer and nanometer length scale. The percolation of the voids and the hydrogen bond network around the voids, may serve as useful order parameters to investigate density fluctuations in supercooled water.