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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Ab Initio Study of the Reaction of Ozone with Bromide Ion
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Ab Initio Study of the Reaction of Ozone with Bromide Ion

机译：臭氧与溴离子反应的从头算研究

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Surface level ozone destruction in polar environments may be initiated by oxidation of bromide ions by ozone, ultimately leading to Br-2 production. Ab initio calculations are used to support the development of atmospheric chemistry models, but errors can occur in study of the bromide-ozone reaction due to inappropriate treatment of the many-electron species and the ionic nature of the reaction. In this work, a high level ab initio study is used to take into account the electronic correlation and the polarization effects. Our results show three possible pathways for the reaction. In particular, we find that this process, though endothermic on the singlet spin state surface, can be energetically feasible on the triplet surface. The triplet surface can be reached through photoexcitation of ozone or by the spin crossing of the potential energy surface. Because this process is known to occur in the dark, it may be that it occurs after intersystem crossing to a triplet surface. This paper also provides a starting point calibration for any future ab initio calculation studies of the bromide-ozone reaction, from the gas to the condensed phase.
机译：极性环境中表面臭氧的破坏可能是由臭氧氧化溴离子引发的，最终导致产生Br-2。从头算可以用来支持大气化学模型的开发，但是由于对多电子物种的处理不当以及反应的离子性质，在溴化物-臭氧反应的研究中可能会出现错误。在这项工作中，使用了一个高水平的从头算研究来考虑电子相关性和极化效应。我们的结果显示了该反应的三种可能途径。特别地，我们发现，尽管在单重态自旋态表面上吸热，但是该过程在三重态表面上在能量上是可行的。可通过臭氧的光激发或势能表面的自旋交叉来达到三重态表面。因为已知此过程是在黑暗中发生的，所以它可能是在系统间交叉到三重态表面之后发生的。本文还为以后从气相到冷凝相的溴-臭氧反应的从头算计算研究提供了一个起点校准。

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