Department of Chemistry and Chemical Biology, Cornell University, Ithaca, New York 14853, USA.
J Chem Phys. 2012 Apr 14;136(14):144105. doi: 10.1063/1.3696963.
We extend the orbital-specific-virtual tensor factorization, introduced for local Møller-Plesset perturbation theory in Ref. [J. Yang, Y. Kurashige, F. R. Manby and G. K. L. Chan, J. Chem. Phys. 134, 044123 (2011)], to local coupled cluster singles and doubles theory (OSV-LCCSD). The method is implemented by modifying an efficient projected-atomic-orbital local coupled cluster program (PAO-LCCSD) described recently, [H.-J. Werner and M. Schütz, J. Chem. Phys. 135, 144116 (2011)]. By comparison of both methods we find that the compact representation of the amplitudes in the OSV approach affords various advantages, including smaller computational time requirements (for comparable accuracy), as well as a more systematic control of the error through a single energy threshold. Overall, the OSV-LCCSD approach together with an MP2 correction yields small domain errors in practical calculations. The applicability of the OSV-LCCSD is demonstrated for molecules with up to 73 atoms and realistic basis sets (up to 2334 basis functions).
我们将局部 Møller-Plesset 微扰理论中引入的轨道特定虚拟张量分解[J. Yang, Y. Kurashige, F. R. Manby 和 G. K. L. Chan, J. Chem. Phys. 134, 044123 (2011)]推广到局部耦合簇单双激发理论（OSV-LCCSD）。该方法通过修改最近描述的高效投影原子轨道局部耦合簇程序（PAO-LCCSD）来实现[H.-J. Werner 和 M. Schütz, J. Chem. Phys. 135, 144116 (2011)]。通过对两种方法的比较，我们发现 OSV 方法中振幅的紧凑表示形式具有各种优势，包括更小的计算时间要求（具有可比的精度），以及通过单个能量阈值更系统地控制误差。总体而言，OSV-LCCSD 方法与 MP2 校正相结合，在实际计算中产生较小的域误差。该 OSV-LCCSD 的适用性已通过具有多达 73 个原子和实际基组（多达 2334 个基函数）的分子得到证明。
