A Full-Dimensional Potential Energy Surface and Dynamics of the Multichannel Reaction between H and HO2.
A Full-Dimensional Potential Energy Surface and Dynamics of the Multichannel Reaction between H and HO2.
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H 和 HO2 之间多通道反应的全维势能面和动力学。
DOI：
10.1021/acs.jpca.0c11213
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发表时间：
2021
期刊：
影响因子：
--
通讯作者：
Jun Li
中科院分区：
文献类型：
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作者：
Jia Li;Jun Li
除了在燃烧和大气化学中的重要意义外，H‘和HO2在基态三重态上的反应代表了一个具有多个产物通道的原型，包括H2+O2、OH+OH、O+H2O和H+H’O2。在这项工作中，建立了标题反应的全维精确势能面(PES)，为所有动力学相关区域提供了可靠的描述。在此基础上，我们采用准经典轨道方法研究了相应的反应动力学，包括各产物通道的反应性和相应的产物支化率、产物能量分布、产物角分布以及相关的微观机理。为了表示产物能量的分布，如产物的平动能以及产物的转动和振动能，使用了传统的直方图和核密度估计(KDE)两种方法并进行了比较。在不同的方法中，这项工作中所得到的分布的特征似乎彼此非常相似。建议使用KDE方法进行统计，特别是对于直方图中波动较小的总体。
In addition to its vital significance in combustion and atmospheric chemistry, the reaction between H' and HO2 on the ground triplet state represents a prototype with multiple product channels, including H2 + O2, OH + OH, O + H2O, and H + H'O2. In this work, a full-dimensional accurate potential energy surface (PES) for the title reaction was developed to provide reliable descriptions for all dynamically relevant regions. Using this PES, we adopted the quasi-classical trajectory approach to study the corresponding reaction dynamics, including the reactivity of each product channel and the associated product branching ratio, the product energy distributions, product angular distributions, and associated microscopic mechanisms. For representing distributions of the product energies, such as product translational energy as well as product rotational and vibrational energies, both the traditional histogram and the kernel density estimation (KDE) methods were used and compared. It seems that the features of the resulting distributions in this work are very similar to each other among different methods. The KDE method is suggested for statistics, particularly for those populations with small oscillations in the histogram plot.