Beyond CCSD(T) Accuracy at Lower Scaling with Auxiliary Field Quantum Monte Carlo.

IF 5.5 1区化学 Q2 CHEMISTRY, PHYSICAL Journal of Chemical Theory and Computation Pub Date : 2025-02-25 Epub Date: 2025-02-05 DOI:10.1021/acs.jctc.4c01314

Ankit Mahajan, James H Thorpe, Jo S Kurian, David R Reichman, Devin A Matthews, Sandeep Sharma

引用次数: 0

Abstract

We introduce a black-box auxiliary field quantum Monte Carlo (AFQMC) approach to perform highly accurate electronic structure calculations using configuration interaction singles and doubles (CISD) trial states. This method consistently provides more accurate energy estimates than coupled cluster singles and doubles with perturbative triples (CCSD(T)), often regarded as the gold standard in quantum chemistry. This level of precision is achieved at a lower asymptotic computational cost, scaling as O(N⁶) compared to the O(N⁷) scaling of CCSD(T). We provide numerical evidence supporting these findings through results for challenging main group and transition metal-containing molecules.

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辅助场量子蒙特卡罗在低尺度下的CCSD(T)精度。

我们引入了一种黑箱辅助场量子蒙特卡罗（AFQMC）方法，利用组态相互作用单双试态（CISD）进行高精度的电子结构计算。这种方法始终提供更准确的能量估计比耦合簇单和双与微扰三重（CCSD(T)），通常被认为是量子化学的黄金标准。与CCSD(T)的0 （N7）缩放相比，这种精度水平以较低的渐近计算成本实现，缩放为O（N6）。我们通过挑战含主族和过渡金属分子的结果提供了支持这些发现的数值证据。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

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Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere.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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