Domain-Based Local Pair Natural Orbital Version of Mukherjee's State-Specific Coupled Cluster Method
Domain-Based Local Pair Natural Orbital Version of Mukherjee's State-Specific Coupled Cluster Method
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DOI：
10.1021/acs.jctc.7b01184
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发表时间：
2018-03-01
影响因子：
5.5
通讯作者：
Demel, Ondrej
中科院分区：
文献类型：
--
作者：
Brabec, Jiri;Lang, Jakub;Demel, Ondrej
本文报告了 Mukherjee 的状态特定多参考耦合聚类方法的局部变体的开发，该方法基于基于域的对自然轨道方法 (DLPNO-MkCC)。当前的实现仅限于连接的单激励和双激励以及具有最多双激励参考的模型空间。 DLPNO-MkCCSD 的性能通过四亚甲基乙烷的计算进行了测试。结果表明，相对于传统的MkCC方法，99.9%以上的相关能量被恢复。为了证明该方法对大型系统的适用性，研究了三角烯和双(1-(2,6-二异丙基苯基)-3,3,5,5-四甲基吡咯烷-2-亚基)铍络合物的单线态三重态能隙。对于最后一个系统（105 个原子），我们能够在不到 9 天的时间内在单个 CPU 上执行具有 2158 个基函数的 cc-pVTZ 计算。
This article reports development of a local variant of Mukherjee's state-specific multireference coupled cluster method based on the domain-based pair natural orbital approach (DLPNO-MkCC). The current implementation is restricted to connected single and double excitations and model space with up to biexcited references. The performance of the DLPNO-MkCCSD was tested on calculations of tetramethyleneethane. The results show that above 99.9% of the correlation energy was recovered, with respect to the conventional MkCC method. To demonstrate the applicability of the method to large systems, singlet triplet gaps of triangulene and bis(1-(2,6-dlisopropylphenyl)-3,3,5,5-tetramethylpyrrolidine-2-ylidene)beryllium complex were studied. For the last system (105 atoms), we were able to perform a calculation in cc-pVTZ with 2158 basis functions on a single CPU in less than 9 days.