从微观模拟自动化发动机获得的水相中四价锕系元素的性质
Properties of the tetravalent actinide series in aqueous phase from a microscopic simulation automated engine
摘要：
在核燃料再循环和环境问题的背景下，用各种方法理解放射性元素的性质仍然是一个挑战。此外，在实验上，必须在足够高的浓度下工作，以达到分析工具的灵敏度，这通常会导致其中一些沉淀，并且稳定某些锕系元素的特定氧化态仍然是一个挑战，因此很难提取整个锕系元素的一般趋势。作为实验的补充，模型可以用来无偏地探测水环境中锕系元素的性质，并提供一个预测工具。我们首次报道了基于均匀力场的分子动力学模拟，对水相中从$\mathrm{Th^{IV}}$到$\mathrm{Bk^{IV}}$并包括$\mathrm{Pu^{IV}}$的整个系列四价锕系元素进行了模拟。用于模拟组分之间相互作用的力场包括极化和电荷捐赠微观效应。它们是由基于自动迭代\textit{ab initio}的引擎构建的，这是未来机器学习过程的核心元素，致力于生成精确的力场。我们模拟的水合锕系元素的性能与现有的实验数据的比较表明，我们的参数分配引擎的模型的鲁棒性和相关性。此外，我们模拟的结构，动力学和水化自由能数据表明，除了$\mathrm{Am^{IV}}$和$\mathrm{Cm^{IV}}$，锕系元素的性质沿系列逐渐变化。
英文摘要：
In the context of nuclear fuel recycling and environmental issues, the understanding of the properties of radio-elements with various approaches remains a challenge regarding their dangerousness. Moreover, experimentally, it is imperative to work at sufficiently high concentrations to reach the sensitivities of the analysis tools, which often leads to precipitation for some of them, and stabilizing of specific oxidation states of some actinides remains a challenge, thus making it difficult to extract general trends across the actinide series. Complementary to experiments, modelling can be used to unbiasedly probe the actinide's properties in aquatic environment and offers a predictive tool. We report the first molecular dynamics simulations based on homogeneously built force fields for the whole series of the tetravalent actinides in aqueous phase from $\mathrm{Th^{IV}}$ to $\mathrm{Bk^{IV}}$ and including $\mathrm{Pu^{IV}}$. The force fields used to model the interactions among the constituents include polarization and charge donation microscopic effects. They are built from an automated iterative \textit{ab initio} based engine, the core element of a future machine learning procedure devoted to generate accurate force fields. The comparison of our simulated hydrated actinide properties to available experimental data show the model robustness and the relevance of our parameter assignment engine. Moreover our simulated structural, dynamical and hydration free energy data show that, apart from $\mathrm{Am^{IV}}$ and $\mathrm{Cm^{IV}}$, the actinides properties change progressively along the series.
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