递归线性张量展开式的自然占用分析。

IF 5.5 1区 化学 Q2 CHEMISTRY, PHYSICAL
Zeynep Gündoğar*, , , Mads Greisen Ho̷jlund*, , , Kasper Green Larsen*, , and , Ove Christiansen*, 
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引用次数: 0

摘要

我们介绍了一种创新的递归张量分解方法,该方法从量子化学理论中汲取灵感。这种方法集成了自然占位数和自然基等思想,就像自然轨道一样,并在构型相互作用理论的线性展开中采用了与激发能级截断平行的截断。该框架的特点是递归算法,将线性展开与每一步的自然基变换相结合,确保收敛到原始张量。因此,开发了一种仅使用有限维的子张量和一系列矩阵变换,在预定公差范围内精确重建初始张量的数值技术。已经为3D张量场景创建了一个初始的Python实现,其中3D张量被分解为单独使用向量和矩阵表示。我们说明了自然基算法中最终递归线性张量展开在处理随机数据集、来自不同来源的实张量和复张量的实验数据集以及代表时间无关和时间相关的水的非谐振动波函数的数据集中的行为。最后,对密度拟合双电子斥力积分的系统精度控制进行了说明,并对氮分子和苯分子的二阶相关能进行了测试。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Recursive Linear Tensor Expansion with Natural Occupation Analysis

Recursive Linear Tensor Expansion with Natural Occupation Analysis

We introduce an innovative recursive tensor decomposition method that draws inspiration from quantum chemical theories. This approach integrates ideas such as natural occupation numbers and natural basis, much like natural orbitals, and employs truncations that parallel the excitation-level truncations in the linear expansions of configuration interaction theory. The framework features recursive algorithms that combine linear expansion with natural basis transformations at each step, ensuring convergence to the original tensor. Consequently, a numerical technique is developed that reconstructs the initial tensor with precision within a predetermined tolerance, using only subtensors of limited dimension and a series of matrix transformations. An initial Python implementation has been created for the 3D tensor scenario where 3D tensors are decomposed to be represented using vectors and matrices alone. We illustrate the behavior of the final Recursive Linear Tensor Expansion in Natural basis algorithm in processing random data sets, experimental data sets from diverse sources with both real and complex tensors, and data sets representing both time-independent and time-dependent anharmonic vibrational wave functions of water. Finally, the systematic accuracy control is illustrated for density fitting two-electron repulsion integrals and tested for the second-order correlation energy of molecular nitrogen and benzene.

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来源期刊
Journal of Chemical Theory and Computation
Journal of Chemical Theory and Computation 化学-物理:原子、分子和化学物理
CiteScore
9.90
自引率
16.40%
发文量
568
审稿时长
1 months
期刊介绍: The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.
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