Geometry optimization and the electronic structure calculations of Pu Z + complexes ( Z = 3–6) in water solution have been performed, within the framework of the DMol 3 and Relativistic Discrete-Variational (RDV) methods. For the simulation of Pu Z + molecular environment in aqueous solution we used 22 and 32 water molecules randomly distributed around cation. To model the effect of bulk solvent environment we used COSMO (Conductor-like Screening Model) potential for water ( ε = 78.54). The obtained results showed that this approach allows the modeling of water dissociation and the formation of hydrolysis products. Our previously suggested scheme for the calculation of interaction energies between selected fragments of multi-molecular systems provides the quantitative estimation of the interaction strengths between plutonium in various oxidation states and each ligand in the first and second coordination shells in water solution.

中文翻译：

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水中的配合物：从头算的新方法

在DMol 3和相对论离散变分（RDV）方法的框架内，已完成了水溶液中Pu Z +配合物（Z = 3–6）的几何优化和电子结构计算。为了模拟水溶液中的Pu Z +分子环境，我们使用了在阳离子周围随机分布的22和32个水分子。为了模拟整体溶剂环境的影响，我们使用了COSMO（类似导体的筛查模型）对水的电势（ε= 78.54）。获得的结果表明，该方法可以模拟水的离解和水解产物的形成。