Optimization methods for finding minimum energy paths
Optimization methods for finding minimum energy paths
复制标题
DOI：
10.1063/1.2841941
复制
发表时间：
2008-04-07
影响因子：
4.4
通讯作者：
Henkelman, Graeme
中科院分区：
文献类型：
--
作者：
Sheppard, Daniel;Terrell, Rye;Henkelman, Graeme
比较了基于状态链的寻找最小能量路径（MEP）的方法。在每种方法中，沿着两个局部最小值之间的初始路径的一组图像被松弛以找到 MEP。我们比较了微移弹性带 (NEB)、双微移弹性带、字符串和简化字符串方法，每种方法都有一组常用的优化器。我们的结果表明，NEB 和字符串方法本质上是等效的，并且在与合适的优化器结合使用时是查找 MEP 的最有效方法。我们发现最有效的优化器是有限内存 Broyden-Fletcher-Goldfarb-Shanno 方法的一种形式，其中为沿路径的所有图像全局构建近似逆 Hessian 矩阵。使用攀爬图像可以找到鞍点，同时用尽可能少的图像表示 MEP。如果需要高精度 MEP，则发现从鞍点下降到最小值比使用具有许多图像的状态链方法更有效。我们的结果基于成对莫尔斯势来模拟 Pt(111) 上七聚体岛的重排，并基于平面波密度泛函理论来模拟 Pd 四聚体在 MgO(100) 上的翻转扩散机制以及氧在 Au(111) 上的解离吸附和扩散。 (C) 2008 年美国物理研究所。
A comparison of chain-of-states based methods for finding minimum energy pathways (MEPs) is presented. In each method, a set of images along an initial pathway between two local minima is relaxed to find a MEP. We compare the nudged elastic band (NEB), doubly nudged elastic band, string, and simplified string methods, each with a set of commonly used optimizers. Our results show that the NEB and string methods are essentially equivalent and the most efficient methods for finding MEPs when coupled with a suitable optimizer. The most efficient optimizer was found to be a form of the limited-memory Broyden-Fletcher-Goldfarb-Shanno method in which the approximate inverse Hessian is constructed globally for all images along the path. The use of a climbing-image allows for finding the saddle point while representing the MEP with as few images as possible. If a highly accurate MEP is desired, it is found to be more efficient to descend from the saddle to the minima than to use a chain-of-states method with many images. Our results are based on a pairwise Morse potential to model rearrangements of a heptamer island on Pt(111), and plane-wave based density functional theory to model a rollover diffusion mechanism of a Pd tetramer on MgO(100) and dissociative adsorption and diffusion of oxygen on Au(111). (C) 2008 American Institute of Physics.