Divide-and-Conquer Linear-Scaling Quantum Chemical Computations
Divide-and-Conquer Linear-Scaling Quantum Chemical Computations
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DOI：
10.1021/acs.jpca.2c06965
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发表时间：
2023-01-11
影响因子：
2.9
通讯作者：
Nishimura，Yoshifumi
中科院分区：
文献类型：
--
作者：
Nakai，Hiromi;Kobayashi，Masato;Nishimura，Yoshifumi
当将量子化学计算应用于更复杂和有吸引力的目标时，碎裂和嵌入方案是非常重要的。基于分而治之（DC）的量子化学模型是一种可以与嵌入方案相连的碎裂方案。这篇专题文章解释了作者在过去二十年中开发的几种基于DC的方案，这些方案受到Yang和Lee（J.Chem.Phys.1995，103，5674-5678）对DC自洽场（SCF）方法的开创性研究的启发。首先，基于DC的SCF，电子相关，激发态，和核轨道方法的理论方面进行了描述，其次是两个组件的相对论理论，量子力学分子动力学模拟，并介绍了三个程序，包括基于DC的计划。说明性的应用程序证实了基于DC的计划的准确性和可行性。
Fragmentation and embedding schemes are of great importance when applying quantum-chemical calculations to more complex and attractive targets. The divide-and-conquer (DC)-based quantum-chemical model is a fragmentation scheme that can be connected to embedding schemes. This feature article explains several DC-based schemes developed by the authors over the last two decades, which was inspired by the pioneering study of DC self-consistent field (SCF) method by Yang and Lee (J. Chem. Phys.1995,103, 5674–5678). First, the theoretical aspects of the DC-based SCF, electron correlation, excited-state, and nuclear orbital methods are described, followed by the two-component relativistic theory, quantum-mechanical molecular dynamics simulation, and the introduction of three programs, including DC-based schemes. Illustrative applications confirmed the accuracy and feasibility of the DC-based schemes.