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首页> 外文期刊>The Journal of Chemical Physics >Nudged elastic band calculations accelerated with Gaussian process regression
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Nudged elastic band calculations accelerated with Gaussian process regression

机译：高斯工艺回归加速了闪烁的弹性带计算

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摘要

Minimum energy paths for transitions such as atomic and/or spin rearrangements in thermalized systems are the transition paths of largest statistical weight. Such paths are frequently calculated using the nudged elastic band method, where an initial path is iteratively shifted to the nearest minimum energy path. The computational effort can be large, especially when ab initio or electron density functional calculations are used to evaluate the energy and atomic forces. Here, we show how the number of such evaluations can be reduced by an order of magnitude using a Gaussian process regression approach where an approximate energy surface is generated and refined in each iteration. When the goal is to evaluate the transition rate within harmonic transition state theory, the evaluation of the Hessian matrix at the initial and final state minima can be carried out beforehand and used as input in the minimum energy path calculation, thereby improving stability and reducing the number of iterations needed for convergence. A Gaussian process model also provides an uncertainty estimate for the approximate energy surface, and this can be used to focus the calculations on the lesser-known part of the path, thereby reducing the number of needed energy and force evaluations to a half in the present calculations. The methodology is illustrated using the two-dimensional Muller-Brown potential surface and performance assessed on an established benchmark involving 13 rearrangement transitions of a heptamer island on a solid surface. Published by AIP Publishing.
机译：热化系统中的原子和/或旋转重排等过渡的最小能量路径是最大统计量的过渡路径。这些路径经常使用闪烁的弹性频带方法计算，其中初始路径迭代地移位到最接近的最小能量路径。计算工作可能很大，特别是当AB Initio或电子密度函数计算用于评估能量和原子力时。这里，我们示出了使用高斯过程回归方法可以通过幅度的数量级来减少这种评估的数量的数量级，其中在每次迭代中产生和精制近似能量表面。当目标是评估谐波过渡状态理论内的过渡率时，可以预先进行初始状态最小值和最终状态最小值的Hessian矩阵的评估，并用作最小能量路径计算中的输入，从而提高稳定性并减少收敛所需的迭代次数。高斯工艺模型还提供了对大致能量表面的不确定性估计，这可以用于将计算聚焦在路径的较小部分上，从而减少所需的能量和力评估到本发明的一半计算。使用二维Muller-棕色电位表面和在实心表面上的结束的基准测试上进行评估的二维Muller-棕色电位表面和性能。通过AIP发布发布。

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