Addressing an instability in unrestricted density functional theory direct dynamics simulations,Journal of Computational Chemistry

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Addressing an instability in unrestricted density functional theory direct dynamics simulations
Journal of Computational Chemistry ( IF 3.4 ) Pub Date : 2018-10-26 , DOI: 10.1002/jcc.25604
Shreyas Malpathak _{1,

2} , Xinyou Ma ₁ , William L. Hase ₁

Affiliation

In Density Functional Theory (DFT) direct dynamics simulations with Unrestricted Hartree Fock (UHF) theory, triplet instability often emerges when numerically integrating a classical trajectory. A broken symmetry initial guess for the wave function is often used to obtain the unrestricted DFT potential energy surface (PES), but this is found to be often insufficient for direct dynamics simulations. An algorithm is described for obtaining smooth transitions between the open‐shell and the closed‐shell regions of the unrestricted PES, and thus stable trajectories, for direct dynamics simulations of dioxetane and its •OCH2‐CH2O• singlet diradical. © 2018 Wiley Periodicals, Inc.

中文翻译：

解决无限制密度泛函理论直接动力学模拟中的不稳定性

在使用无限制哈特里福克 (UHF) 理论的密度泛函理论 (DFT) 直接动力学模拟中，在对经典轨迹进行数值积分时，经常会出现三重态不稳定性。波函数的破坏对称性初始猜测通常用于获得不受限制的 DFT 势能面 (PES)，但发现这通常不足以直接进行动力学模拟。描述了一种算法，用于获得不受限制的 PES 的开壳和闭壳区域之间的平滑过渡，从而获得稳定的轨迹，用于二氧杂环丁烷及其 •OCH2-CH2O• 单线态双自由基的直接动力学模拟。© 2018 威利期刊公司。

更新日期：2018-10-26

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