ChemDyME：通过组合分子动力学和主方程计算的动力学操纵的自动机构生成
ChemDyME: Kinetically Steered, Automated Mechanism Generation Through Combined Molecular Dynamics and Master Equation Calculations
摘要：
在许多科学领域，人们都有兴趣了解复杂化学网络的演化方式。研究人员关注的化学网络变得越来越复杂，这促使开发了以黑盒方式探索化学反应性或构象变化的自动化方法，利用现代计算资源来自动化机制发现。在这项工作中，我们提出了一种新的方法来实现自动化机制生成耦合分子动力学和统计速率理论，自动找到动力学上重要的反应，然后解决在不断发展的网络中的物种的时间演化。这种ChemDyME方法的关键是动力学收敛的新概念，从而将对新反应的搜索限制在那些在感兴趣的条件下动力学上有利的物种上。我们证明了两个系统的新方法的能力，一个研究充分的燃烧系统，和一个多个氧气添加系统相关的大气气溶胶的形成。
英文摘要：
In many scientific fields, there is an interest in understanding the way in which complex chemical networks evolve. The chemical networks which researchers focus upon, have become increasingly complex and this has motivated the development of automated methods for exploring chemical reactivity or conformational change in a black box manner, harnessing modern computing resources to automate mechanism discovery. In this work we present a new approach to automated mechanism generation implemented which couples molecular dynamics and statistical rate theory to automatically find kinetically important reactions and then solve the time evolution of the species in the evolving network. Key to this ChemDyME approach is the novel concept of kinetic convergence whereby the search for new reactions is constrained to those species which are kinetically favorable at the conditions of interest. We demonstrate the capability of the new approach for two systems, a well-studied combustion system, and a multiple oxygen addition system relevant to atmospheric aerosol formation.
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