论文标题
用于大型系统的精确远处校正的全分子局部局部相关方法
The Cluster-in-Molecule Local Correlation Method with an Accurate Distant Pair Correction for Large Systems
论文作者
论文摘要
提出了具有准确的远处相关能校正的局部分子（CIM）局部相关方法。对于大型系统，包括遥远的对相关能量对于绝对相关能和相对能量的准确预测至关重要。在这里，我们提出了一个简单有效的方案，用于评估遥远的对相关能量校正。可以从集群的电子相关计算中轻易提取校正，而几乎没有额外的努力。基准计算表明，改进的CIM方法可以恢复超过99.97％的常规相关能量。通过将CIM方法与基于域的局部对天然轨道（DLPNO）局部相关方法相结合，我们在CIM-DLPNO-CCSD（T）水平上提供了由八个弱结合的复合物组成的测试集的准确结合能，该测试集的大小为200至1027个原子。通过这些结果作为参考数据，已经评估了其他电子相关方法的准确性和适用性和大型系统的一些密度功能方法。
The cluster-in-molecule (CIM) local correlation approach with an accurate distant pair correlation energy correction is presented. For large systems, the inclusion of distant pair correlation energies is essential for the accurate predictions of absolute correlation energies and relative energies. Here we propose a simple and efficient scheme for evaluating the distant pair correlation energy correction. The corrections can be readily extracted from electron correlation calculations of clusters with almost no additional effort. Benchmark calculations show that the improved CIM approach can recover more than 99.97% of the conventional correlation energy. By combining the CIM approach with the domain based local pair natural orbital (DLPNO) local correlation approach, we have provided accurate binding energies at the CIM-DLPNO-CCSD(T) level for a test set consisting of eight weakly bound complexes ranging in size from 200 to 1027 atoms. With these results as the reference data, the accuracy and applicability of other electron correlation methods and a few density functional methods for large systems have been assessed.
