Spontaneous nucleation in water is challenging to study in molecular simulations due to its stochastic nature.  Often it is left to open ended sampling with the hope that potential nucleation centers are able to survive essentially random particle collisions, these in addition to the constant thermal and volumetric fluctuations inherent in systems sampling at constant temperature and pressure.  Motivated by spontaneous crystallization observations using Molecular Dynamics simulations of a two-dimensional water-like model, we have investigated hydrogen-bond organization signatures giving rise to spontaneous nucleation.  Sitting on the solid-liquid phase boundary line, we track dynamic and complete water crystallization and melting events from single nucleation clusters all the way to extended connected ring networks in 2D.  We extend these investigations to the third-dimension by identifying analogous 3D water nucleation signatures in a post-simulation hydrogen-bond connectivity analysis.  Tracking the connectivity distributions as a function of simulation state provides unique insight into organization in disordered liquid and supercooled water as well as insight into the driving forces in water nucleation and crystallization.

Nucleation tracking in aqueous environments

255th National Meeting (2018)

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.