Bootstrap Embedding For Large Molecular Systems
Bootstrap Embedding For Large Molecular Systems
复制标题
大分子系统的自举嵌入
DOI：
10.1021/acs.jctc.0c00438
复制
发表时间：
2020
影响因子：
5.5
通讯作者：
Van Voorhis, Troy
中科院分区：
文献类型：
--
作者：
Ye, Hong-Zhou;Tran, Henry K.;Van Voorhis, Troy
量子嵌入理论的最新发展为大系统的关联计算提供了有吸引力的方法。在这项工作中，我们扩展了我们以前的工作[J. Chem. Theory Comput.2019，15，4497-4506; J. Phys. Chem. Lett.2019，10，6368-6374]关于自举嵌入（BE）的工作，以实现大分子在耦合簇单双（CCSD）水平上的相关从头计算。我们介绍了几个新的算法的发展，显着降低BE的计算成本，同时保持其准确性。最后的实现对于积分变换阿索（N3），对于CCSD计算为O（N）。一系列共轭分子的数值结果表明，BE与合理大小的片段可以恢复超过99.5%的总相关能量的一个完整的CCSD计算，而所需的计算资源（时间和存储）比较有利的一个流行的本地相关计划：域本地化对自然轨道（DLPNO）。在这项工作中，最大的BE计算涉及到2900个基函数，并且可以在几天内在具有16个CPU核心和64 GB内存的单个节点上执行。我们预计，这些发展代表了重要的一步，应用BE解决实际问题。
Recent developments in quantum embedding theories have provided attractive approaches to correlated calculations for large systems. In this work, we extend our previous work [J. Chem. Theory Comput.2019,15, 4497–4506;J. Phys. Chem. Lett.2019,10, 6368–6374] on bootstrap embedding (BE) to enable correlated ab initio calculations at the coupled cluster with singles and doubles (CCSD) level for large molecules. We introduce several new algorithmic developments that significantly reduce the computational cost of BE, while maintaining its accuracy. The resulting implementation scales asO(N3) for the integral transform andO(N) for the CCSD calculation. Numerical results on a series of conjugated molecules suggest that BE with reasonably sized fragments can recover more than 99.5% of the total correlation energy of a full CCSD calculation, while the required computational resources (time and storage) compare favorably to one popular local correlation scheme: domain localized pair natural orbital (DLPNO). The largest BE calculation in this work involves ∼2900 basis functions and can be performed on a single node with 16 CPU cores and 64 GB of memory in a few days. We anticipate that these developments represent an important step toward the application of BE to solve practical problems.