论文标题
水 - 离子簇中的自我交流校正
Self-Interaction Correction in Water-Ion Clusters
论文作者
论文摘要
我们研究了各种水簇在密度功能近似中的自我交互误差的重要性。我们采用了与LSDA，PBE和SCAN结合使用的Fermi-Löwdin轨道自我交织校正（FLOSIC）方法来描述氢键含水的水簇簇的结合能，\ \ textit {即。在氢键的水离子簇中，构建块由氢原子连接，尽管这些链接比水分子之间的正常氢键更强，较长，因为离子上的单子与水分子上的永久性和诱导的偶极子相互作用。我们发现，自我交织误差超越了氢键的水簇簇，这会减少误差，并使结合能与更高级别的计算更紧密地一致。非氢键水 - 阿尔卡利群集没有显着影响自我相互作用误差。自我交互校正的PBE预测，在结合能（$ \ leq $ 50 MEV/\ CE {H2O}）中，最低的平均无符号误差对于氢键键入的水簇。自我交流误差也很大程度上取决于群集的大小，而Flosic并未准确捕获所有簇中的细微变化，表明需要进一步细化。
We study the importance of self-interaction errors in density functional approximations for various water-ion clusters. We have employed the Fermi-Löwdin orbital self-interaction correction (FLOSIC) method in conjunction with LSDA, PBE, and SCAN to describe binding energies of hydrogen-bonded water-ion clusters, \textit{i.e.}, water-hydronium, water-hydroxide, water-halide, as well as non-hydrogen-bonded water-alkali clusters. In the hydrogen-bonded water-ion clusters, the building blocks are linked by hydrogen atoms, although the links are much stronger and longer-ranged than the normal hydrogen bonds between water molecules, because the monopole on the ion interacts with both permanent and induced dipoles on the water molecules. We find that self-interaction errors overbind the hydrogen-bonded water-ion clusters and that FLOSIC reduces the error and brings the binding energies into closer agreement with higher-level calculations. The non-hydrogen-bonded water-alkali clusters are not significantly affected by self-interaction errors. Self-interaction corrected PBE predicts the lowest mean unsigned error in binding energies ($\leq$ 50 meV/\ce{H2O}) for hydrogen-bonded water-ion clusters. Self-interaction errors are also largely dependent on the cluster size, and FLOSIC does not accurately capture the subtle variation in all clusters, indicating the need for further refinement.
