发表机构
University of Stuttgart; Dipartimento di Chimica e Chimica Industriale（斯图加特大学; 化学与工业化学系）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本文提出一种振幅外推ansatz，利用先前几何步的计算为拟牛顿求解器提供初始猜测，加速耦合簇和Lambda求解器收敛，并在中等尺寸分子上显著减少迭代次数。
AI 中文摘要
在这项工作中，我们提出了一种用于几何优化的振幅外推ansatz，它利用先前步骤的计算来为每个新几何处的拟牛顿求解器构造初始猜测，从而显著加速耦合簇和Lambda求解器的收敛。该ansatz包含必要的振幅变换，以减轻在Hartree-Fock理论水平上轨道能量交叉引起的不连续性，同时保持计算和内存效率。该方法在一组多样化的中等尺寸分子上进行了测试，证明与常规方法相比，耦合簇迭代次数有系统性的显著减少。
英文摘要
In this work, we present an amplitude extrapolation ansatz for geometry optimization that uses calculations from previous steps to construct an initial guess for the quasi-Newton solver at each new geometry, significantly accelerating convergence of the coupled-cluster and Lambda solver alike. The ansatz incorporates a necessary amplitude transformation to mitigate discontinuities associated with orbital energy crossings at the Hartree-Fock level of theory, while remaining computational and memory efficient. The method is tested for a diverse set of medium-sized molecules to demonstrate a systematic and significant reduction in the number of coupled-cluster iterations compared to the conventional method.
CommentsMain article 17 pages, 4 figures, 1 table. Supplementary material 6 pages, 7 figues, 1 table
