Automated Discovery of Elementary Chemical Reaction Steps Using Freezing String and Berny Optimization Methods
Automated Discovery of Elementary Chemical Reaction Steps Using Freezing String and Berny Optimization Methods
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DOI：
10.1021/acs.jctc.5b00407
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发表时间：
2015-09-01
影响因子：
5.5
通讯作者：
Green, William H.
中科院分区：
文献类型：
--
作者：
Suleimanov, Yury V.;Green, William H.
我们提出了一个简单的协议，它允许全自动发现基本化学反应步骤，合作分别使用双端和单端过渡态优化算法冻结字符串和Bemy优化方法。为了证明所提出的方法的实用性，研究了燃烧和大气化学重要性的几个单分子体系的反应性。所提出的算法使我们能够在没有任何人为干预的情况下，不仅检测到在以前的研究中手动检测到的“已知”反应路径，而且还检测到涉及重大原子重排的新的、以前“未知”的反应路径。我们相信，将这种系统的方法应用于基元反应路径寻找将极大地加速新化学的发现，并将导致对各种化学过程的更准确的计算机模拟。
We present a simple protocol which allows fully automated discovery of elementary chemical reaction steps using in cooperation double- and single-ended transition-state optimization algorithms the freezing string and Bemy optimization methods, respectively. To demonstrate the utility of the proposed approach, the reactivity of several single-molecule systems of combustion and atmospheric chemistry importance is investigated. The proposed algorithm allowed us to detect without any human intervention not only "known" reaction pathways, manually detected in the previous studies, but also new, previously "unknown", reaction pathways which involve significant atom rearrangements. We believe that applying such a systematic approach to elementary reaction path finding will greatly accelerate the discovery of new chemistry and will lead to more accurate computer simulations of various chemical processes.