论文标题
区域嵌入使表面科学的高级量子化学能力
Regional Embedding Enables High-Level Quantum Chemistry for Surface Science
论文作者
论文摘要
与常见的密度函数相比，初始波函数方法可以提供更大的可靠性和准确性，这在对吸附物进行建模或原本周期系统的缺陷进行建模时可能很有用。然而，翻译对称性的破裂需要大型超级单元，这些超细胞通常对于相关波函数方法而言通常是刺激性的。作为替代方案，我们介绍了区域嵌入方法，该方法仅通过使用简单的重叠标准构建的小，碎片 - 定位的轨道空间来实现仅感兴趣的目标片段的相关波函数处理。在氢化锂，六角硼和石墨烯底物上的吸附上的应用表明，与焦点校正结合的区域嵌入可以提供融合的CCSD（T）（耦合簇）吸附能量，具有很小的碎片尺寸。
Compared to common density functionals, ab initio wave function methods can provide greater reliability and accuracy, which could prove useful when modeling adsorbates or defects of otherwise periodic systems. However, the breaking of translational symmetry necessitates large supercells that are often prohibitive for correlated wave function methods. As an alternative, we introduce the regional embedding approach, which enables correlated wave function treatments of only a target fragment of interest through small, fragment-localized orbital spaces constructed using a simple overlap criterion. Applications to the adsorption of water on lithium hydride, hexagonal boron nitride, and graphene substrates show that regional embedding combined with focal point corrections can provide converged CCSD(T) (coupled cluster) adsorption energies with very small fragment sizes.
