A fast tomographic method for searching the minimum free energy path.
A fast tomographic method for searching the minimum free energy path.
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DOI：
10.1063/1.4897983
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发表时间：
2014-10
期刊：
影响因子：
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通讯作者：
Changjun Chen;Yanzhao Huang;Xuewei Jiang;Yi Xiao
中科院分区：
文献类型：
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作者：
Changjun Chen;Yanzhao Huang;Xuewei Jiang;Yi Xiao
最小自由能路径(MFEP)提供了许多关于化学反应的重要信息，如自由能垒、过渡态的位置以及反应物和产物之间的相对稳定性。利用MFEP，可以有效地研究反应机理。由于自由度较多，搜索MFEP是一个非常耗时的过程。在这里，我们提出了一种快速层析成像方法来执行搜索。我们的方法首先计算垂直于过渡路径的一系列超平面中的自由能表面。基于目标函数和自由能梯度，在集合变量空间迭代优化过渡路径。该方法在系统建模中的应用表明，该方法是实用的。它可以是寻找状态到状态MFEP的另一种方法。
Minimum Free Energy Path (MFEP) provides a lot of important information about the chemical reactions, like the free energy barrier, the location of the transition state, and the relative stability between reactant and product. With MFEP, one can study the mechanisms of the reaction in an efficient way. Due to a large number of degrees of freedom, searching the MFEP is a very time-consuming process. Here, we present a fast tomographic method to perform the search. Our approach first calculates the free energy surfaces in a sequence of hyperplanes perpendicular to a transition path. Based on an objective function and the free energy gradient, the transition path is optimized in the collective variable space iteratively. Applications of the present method to model systems show that our method is practical. It can be an alternative approach for finding the state-to-state MFEP.