Chemoton 2.0: Autonomous Exploration of Chemical Reaction Networks
Chemoton 2.0: Autonomous Exploration of Chemical Reaction Networks
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DOI：
10.1021/acs.jctc.2c00193
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发表时间：
2022-09-13
影响因子：
5.5
通讯作者：
Reiher, Markus
中科院分区：
文献类型：
--
作者：
Unsleber, Jan P.;Grimmel, Stephanie A.;Reiher, Markus
在硬件和算法设计进步的推动下，对化学反应空间的大规模自动化探索已经成为可能。在这里，我们提出了一个开源的、可扩展的框架，用于探索基于量子力学第一原理的化学反应机制。它旨在促进各种化学问题的反应网络探索，具有广泛的目标，如机制阐明，反应路径优化，反合成路径验证，试剂设计和微动力学建模。我们的框架中所有算法严格的第一原理基础是避免对特定化学系统的任何限制的一般适用性的关键。这样的敏捷框架需要多个专门的软件组件，我们在本文中介绍了三个模块。关键模块CHEMOTON驱动对反应网络的探索。对于探索本身，我们引入了两种基于牛顿轨迹的初级步搜索新算法。这些算法的性能评估了各种反应的特点是广泛的化学多样性的键模式和化学元素。CHEMOTON成功地回收了其中的绝大多数。我们提供了结果数据，包括大量未包括在我们的参考集中的反应，作为进一步探索和未来参考的起点。
Fueled by advances in hardware and algorithm design, large-scale automated explorations of chemical reaction space have become possible. Here, we present our approach to an open-source, extensible framework for explorations of chemical reaction mechanisms based on the first-principles of quantum mechanics. It is intended to facilitate reaction network explorations for diverse chemical problems with a wide range of goals such as mechanism elucidation, reaction path optimization, retrosynthetic path validation, reagent design, and microkinetic modeling. The stringent first-principles basis of all algorithms in our framework is key for the general applicability that avoids any restrictions to specific chemical systems. Such an agile framework requires multiple specialized software components of which we present three modules in this work. The key module, CHEMOTON, drives the exploration of reaction networks. For the exploration itself, we introduce two new algorithms for elementary-step searches that are based on Newton trajectories. The performance of these algorithms is assessed for a variety of reactions characterized by a broad chemical diversity in terms of bonding patterns and chemical elements. CHEMOTON successfully recovers the vast majority of these. We provide the resulting data, including large numbers of reactions that were not included in our reference set, to be used as a starting point for further explorations and for future reference.