Citation: Gao Tao, Wang Hong-Yan, Huang Zheng, Zhu Zheng-He, Sun Ying, Wang Xiao-Lin, Fu Yi-Bei. Many-body Expanded Analytical Potential Energy Function for the Ground State of PuO2 Molecule[J]. Acta Physico-Chimica Sinica, 1999, 15(12): 1082-1087. doi: 10.3866/PKU.WHXB19991206
从导出基态PuO2分子的电子状态X5Σg+正确地判断其离解极限出发, 采用MP2方法, 应用相对论有效原子实模型(RECP)优化出PuO2(X5Σg +)分子稳定构型为线性O-Pu-O(D∞h), 其平衡核间距Re=0.18004nm. 同时也计算出振动频率, 并优化出存在亚稳态的Pu-O-O(C∞v)构型. 使用多体项展式理论方法, 导出了基态PuO2分子的分析势能函数. 该势能表面准确地再现了O-Pu-O(D∞h)平衡结构和亚稳态的Pu-O-O(C∞v)构型. 然后根据势能函数等值图讨论了O(3Pg)+PuO反应的势能面静态特征.
Many-body Expanded Analytical Potential Energy Function for the Ground State of PuO2 Molecule
The ground electronic state X 5Σ + g and the reasonable dissociation limits of the PuO2 molecule are derived based on the Atomic and Molecular Reactive Statics. In the MP2 (The HF calculation followed by a second-order Moller-Plesset correlation) level, using the RECP(relativistic effective core potential) for Pu atom and 6 311G* basis for O atom , the present work has optimized the equilibrium geometry for the linear O-Pu-O( D ∞h ), ground state X 5Σg + of PuO2, whose equilibrium nuclear distance and dissociation energy are 0.180 04nm and 12.551 eV respectively. And the metastable structure Pu-O-O( C ∞v )is found for the first time, which is 6.79 eV higher than the stable structure. The analytical potential energy function for the ground state X 5Σg + of PuO 2 has also been derived using many body expansion method, the potential energy function is successfully used for describing the equilibrium geometry of PuO 2 and PuOO, which is adequately accurate in the whole region for the dynamical research.
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