Quantum-Classical Adaptive Resolution Simulations of Aqueous Solvation: Effects of Hydrogen Spatial Delocalization

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Relevant properties of water in the first solvation shell of thefullerene have been shown in our previous work to be deemed local.However, classical models of water tend to provide a solvation structurefar too rigid compared to quantum model based on the spatialdelocalization of atoms in space.As a consequence, while it can be concluded that the general mechanismof aggregation of fullerene molecules in water, being a water-mediatedprocess, requires that the molecules come very close before they feelthe reciprocal presence, the barrier for the formation of a uniquesolvation shell that includes two fullerene molecules differsconsiderably on whether a quantum or a classical model is used. Theadaptive resolution simulation technique (AdResS) by drasticallyremoving the hydrogen bonding degrees of freedom turned out to be apowerful method for reaching such conclusions. Next, with the use of thesame technique, one may extend the study to a non-equilibrium situationwhere an external electric field may either break or strengthen furtherthe properties of locality of water and thus manipulate the behaviour ofthe hydrogen bonding network. This in turn implies to found an optimalexternal (physical) manipulation of the aggregation process in order toobtain a particular wished result (aggregation/non-aggregation).