Pu-H2相互作用的反应机理及电子密度分析

通过量子力学中密度泛函理论的相关方法和相对论有效原子实模型(RECP)，应用Gaussian09程序对钚与氢气的相互作用进行了计算和分析。计算得到了钚与氢气的详细微观反应机理：Pu+H2→FC→TS→PuH2，优化了沿反应路径的特殊结构（能量极小点及过渡态），并通过能量分析画出了势能剖面图。基于优化的几何结构，通过多种拓扑分析方法分析了反应路径中所有特殊结构的电子密度相关性质，如自旋密度分析、Mulliken自旋布居分析、电子定域泛函理论分析，得到了电子密度在反应过程中的详细变化。

Study on Reaction Mechanism and Electron Density of Plutonium-hydrogen Interaction

The interaction between the plutonium atom and hydrogen molecule was calculated and analyzed by using the density functional theory (DFT) and the relativistic effective core potential (RECP) with Gaussian09 program. Due to the special electronic structure of the plutonium atom, it is possible to have multiplet cross in the reaction pathway, so the multiplets of the plutonium atom were considered in calculation. The detailed microscopic reaction process of plutonium atom and hydrogen molecule was calculated as Pu+H₂→FC→TS→PuH₂. The whole reaction process was carried out in the septet state. That is, the reactants, the initial complex, the transition state and the final reaction product in the reaction process are all in septet state. The special structure of the energy minimum points and transition states along the reaction pathway was optimized, and the potential energy profile for energy analysis was drawn. The results of the study are helpful to understand the microscopic reaction process of plutonium atom and hydrogen molecule.