Abstract
| - The process by which supercooled fluids form stable, crystalline solids has been found to beelusive both experimentally and via computer simulations. This is because this process, generally callednucleation, is statistical in nature and because the set of intermediate states, generally called the criticalnucleus, is very short-lived. Thus, there are very large uncertainties in even the limited experimental datathat exist, and computer simulations that have been performed can yield descriptive information at best.Here we present a detailed and quantitatively accurate observation of the most important nucleation process,the freezing of liquid water at ambient conditions. We have accomplished this by using a method based onchoosing a suitable set of order parameters to characterize the crystallinity of the system and a non-Boltzmann sampling Monte Carlo approach to obtain a statistical average of the properties of the systemduring its transition from liquid to ice (Ih). We have characterized the order of the system statistically atintermediate states between liquid water and ice Ih and in so doing described the nucleation process.
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