Considering Density Functional Approaches for Actinide Species: The An66 Molecule Set
Considering Density Functional Approaches for Actinide Species: The An66 Molecule Set
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DOI：
10.1021/acs.jpca.1c06155
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发表时间：
2021-08-09
影响因子：
2.9
通讯作者：
Wilson, Angela K.
中科院分区：
文献类型：
--
作者：
Aebersold, Lucas E.;Wilson, Angela K.
自旋-轨道效应对锕系化合物能量性质预测的重要性已被认为是18种不同的密度泛函，比较自旋-轨道和非自旋-轨道（“标准”）形式的密度泛函理论（DFT）。本文研究了66个小锕系元素（Th-Am）化合物的一组生成谱，即An 66组，已有实验数据。这一系列元素包括锕系元素的卤化物、氧化物和氧卤化物，一般形式为AnO（m）X（n），其中n = 0-6，m = 0-3，X = F、Cl、Br或I。基组选择的影响进行了研究，并帮助帐户的相对论的影响，斯图加特一般和分段收缩原子自然轨道（ANO）基组配对小核心相对论有效核心势（RECP）以及全电子计算利用三阶道格拉斯-克罗尔-赫斯被认为是。
The importance of spin-orbit effects on the predictions of energetic properties of actinide compounds has been considered for 18 different density functionals, comparing the spin-orbit and non-spin-orbit ("standard") forms of density functional theory (DFT). A set of enthalpies of formation for 66 small actinide (Th-Am) compounds-the An66 set, for which experimental data are available-have been investigated. The set includes actinide halides, oxides, and oxohalides in the general form AnO(m)X(n), where n = 0-6, m = 0-3, and X = F, Cl, Br, or I. The impact of basis set choice was investigated, and to help account for the impact of relativity, the Stuttgart general and segmented contracted atomic natural orbital (ANO) basis sets paired with small core relativistic effective core potentials (RECP) as well as all-electron calculations utilizing the third-order Douglas-Kroll-Hess were considered.