Simulating ice nucleation, one molecule at a time, with the ‘DFT microscope’

Abstract

Few physical processes are as ubiquitous as the nucleation of water into ice. However, ice nucleation and, in particular, heterogeneously catalyzed nucleation remains poorly understood at the atomic level. Here, we report an initial series of density functional theory (DFT) calculations aimed at putting our understanding of ice nucleation and water clustering at metallic surfaces on a firmer footing. Taking a prototype hydrophobic metal surface, Cu(111), for which scanning tunneling microscopy measurements of water clustering have recently been performed, possible structures of adsorbed clusters comprised of 2–6 H₂O molecules have been computed. How the water clusters in this size regime differ from those in the gas phase is discussed, as is the nature of their interaction with the substrate.