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

水在富勒烯第一层溶剂化壳层中的相关性质在我们以前的工作中被认为是局域的.然而，与基于空间原子离域的量子模型相比，水的经典模型往往提供的溶剂化结构过于严格.因此，虽然可以得出结论，富勒烯分子在水中聚集的一般机制是水介导的过程，要求分子在感觉到相互存在之前非常接近，形成包括两个富勒烯分子的独特溶剂化壳的屏障在使用量子模型还是经典模型时有很大不同。自适应分辨率模拟技术（AdResS）通过大幅去除氢键自由度而被证明是得出这样的结论的一种强有力的方法。接下来，使用同样的技术，可以将研究扩展到非平衡状态，在这种状态下，外部电场可以进一步破坏或加强水的局域性，从而操纵氢键网络的行为。这反过来又意味着找到一个最佳的外部（物理）操纵的聚集过程，以获得一个特定的希望的结果（聚集/非聚集）。

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).