On the interactions between atmospheric radicals and cloud droplets: A molecular picture of the interface
On the interactions between atmospheric radicals and cloud droplets: A molecular picture of the interface
复制标题
关于大气自由基和云滴之间的相互作用：界面的分子图片
DOI：
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发表时间：
2003
影响因子：
11.1
通讯作者：
S. Kais
中科院分区：
文献类型：
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作者：
Q. Shi;S. D. Belair;J. S. Francisco;S. Kais
几十年来，气相物质如何与云滴结合一直是一个有趣的课题，人们已经做了大量的工作来了解闭合壳层分子和液态水之间的相互作用。然而，开壳层自由基物种和液相云滴之间的相互作用还没有得到很好的理解。为了探测这些相互作用，我们使用量子化学计算来预测的氢过氧自由基（HO2）在（H2O）20球形水笼的存在下的能量。我们的计算表明，它是积极的自由基结合到笼外有利。这种构型具有自由基的氢和末端氧作为其主要键合位点。自由能计算表明，在大气条件下，将有一个分区之间的HO2自由基，表面结合和HO2自由基，溶解到散装。这可能对我们理解自由基化学有重要的影响，并可能使我们深入了解云和气溶胶在大气化学过程中的作用。
How gas-phase materials become incorporated with cloud droplets has been an intriguing subject for decades, and considerable work has been done to understand the interactions between closed-shell molecules and liquid water. The interactions between open-shell radical species and liquid-phase cloud droplets, however, are not well understood. To probe these interactions we used quantum chemistry calculations to predict the energetics of the hydroperoxy radical (HO2) in the presence of an (H2O)20 spherical water cage. Our calculations show that it is energetically favorable for the radical to bind to the outside of the cage. This configuration has the hydrogen and the terminal oxygen of the radical as its primary bonding sites. Free-energy calculations suggest that, at atmospheric conditions, there will be a partitioning between HO2 radicals that are surface-bound and HO2 radicals that dissolve into the bulk. This may have important ramifications for our understanding of radical chemistry and may lend insight into the role that clouds and aerosols play in atmospheric chemical processes.