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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Implementation of dynamical nucleation theory effective fragment potentials method for modeling aerosol chemistry
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Implementation of dynamical nucleation theory effective fragment potentials method for modeling aerosol chemistry

机译：动态成核理论有效碎片势方法在气溶胶化学建模中的实现

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In this work, the dynamical nucleation theory (DNT) model using the ab initio based effective fragment potential (EFP) is implemented for evaluating the evaporation rate constant and molecular properties of molecular clusters. Predicting the nucleation rates of aerosol particles in different chemical environments is a key step toward understanding the dynamics of complex aerosol chemistry. Therefore, molecular scale models of nanoclusters are required to understand the macroscopic nucleation process. On the basis of variational transition state theory, DNT provides an efficient approach to predict nucleation kinetics. While most DNT Monte Carlo simulations use analytic potentials to model critical sized clusters, or use ab initio potentials to model very small clusters, the DNTEFP Monte Carlo method presented here can treat up to critical sized clusters using the effective fragment potential (EFP), a rigorous nonempirical intermolecular model potential based on ab initio electronic structure theory calculations, improvable in a systematic manner. The DNTEFP method is applied to study the evaporation rates, energetics, and structure factors of multicomponent clusters containing water and isoprene. The most probable topology of the transition state characterizing the evaporation of one water molecule from a water hexamer at 243 K is predicted to be a conformer that contains six hydrogen bonds, with a topology that corresponds to two water molecules stacked on top of a quadrangular (H_2O)_4 cluster. For the water hexamer in the presence of isoprene, an increase in the cluster size and a 3-fold increase in the evaporation rate are predicted relative to the reaction in which one water molecule evaporates from a water hexamer cluster.
机译：在这项工作中，使用基于从头算的有效片段电势（EFP）的动态成核理论（DNT）模型用于评估蒸发速率常数和分子簇的分子特性。预测不同化学环境中气溶胶颗粒的成核速率是理解复杂气溶胶化学动力学的关键一步。因此，需要纳米团簇的分子尺度模型来理解宏观成核过程。在变分过渡状态理论的基础上，DNT提供了一种预测成核动力学的有效方法。尽管大多数DNT蒙特卡洛模拟都使用分析势来建模临界大小的簇，或者使用从头算势来建模非常小的簇，但此处介绍的DNTEFP蒙特卡洛方法可以使用有效片段势（EFP）来处理临界大小的簇。基于从头算电子结构理论计算得出的严格的非经验分子间模型潜能，可以系统地改进。 DNTEFP方法用于研究包含水和异戊二烯的多组分簇的蒸发速率，能量学和结构因子。预测过渡态最可能的拓扑特征是一个水分子在243 K时从六聚体中蒸发的特征，被预测为包含六个氢键的构象异构体，其拓扑结构对应于堆叠在四边形顶部的两个水分子（ H_2O）_4群集。对于在异戊二烯存在下的水六聚体，相对于其中一个水分子从水六聚体簇中蒸发的反应，预测了团簇尺寸的增加和蒸发速率的3倍的增加。

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