Ye Hong-Zhou, Berkelbach Timothy C
Department of Chemistry, Columbia University, New York, New York 10027, United States.
Initiative for Computational Catalysis, Flatiron Institute, New York, New York 10010, United States.
J Chem Theory Comput. 2024 Oct 22;20(20):8948-8959. doi: 10.1021/acs.jctc.4c00936. Epub 2024 Oct 8.
We describe the implementation details of periodic local coupled-cluster theory with single and double excitations (CCSD) and perturbative triple excitations [CCSD(T)] using local natural orbitals (LNOs) and -point symmetry. We discuss and compare several choices for orbital localization, fragmentation, and LNO construction. By studying diamond and lithium, we demonstrate that periodic LNO-CC theory can be applied with equal success to both insulators and metals, achieving speedups of 2 to 3 orders of magnitude even for moderately sized -point meshes. Our final predictions of the equilibrium cohesive energy, lattice constant, and bulk modulus for diamond and lithium are in good agreement with previous theoretical predictions and experimental results.
我们描述了使用局域自然轨道（LNO）和点群对称性的含单双激发（CCSD）及微扰三激发[CCSD(T)]的周期性局域耦合簇理论的实现细节。我们讨论并比较了轨道定域化、碎片化和LNO构建的几种选择。通过研究金刚石和锂，我们证明周期性LNO-CC理论可以同样成功地应用于绝缘体和金属，即使对于中等大小的点群网格，也能实现2到3个数量级的加速。我们对金刚石和锂的平衡结合能、晶格常数和体模量的最终预测与先前的理论预测和实验结果高度吻合。
