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Isoprene oxidation mechanisms: measurements and modelling of OH and HO2 over a South-East Asian tropical rainforest during the OP3 field campaign

机译:异戊二烯氧化机制:在OP3野战活动期间,在东南亚热带雨林中测量和建模OH和HO2

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摘要

Forests are the dominant source of volatile organic compounds into the atmosphere, with isoprene being the most significant species. The oxidation chemistry of these compounds is a significant driver of local, regional and global atmospheric composition. Observations made over Borneo during the OP3 project in 2008, together with an observationally constrained box model are used to assess our understanding of this oxidation chemistry. In line with previous work in tropical forests, we find that the standard model based on MCM chemistry significantly underestimates the observed OH concentrations. Geometric mean observed to modelled ratios of OH and HO2 in airmasses impacted with isoprene are 5.324.43+3.68 and 1.180.30+0.30 respectively, with 68 % of the observations being within the specified variation. We implement a variety of mechanistic changes into the model, including epoxide formation and unimolecular decomposition of isoprene peroxy radicals, and assess their impact on the model success. We conclude that none of the current suggestions can simultaneously remove the bias from both OH and HO2 simulations and believe that detailed laboratory studies are now needed to resolve this issue.
机译:森林是挥发性有机化合物进入大气中的主要来源,其中异戊二烯是最重要的物种。这些化合物的氧化化学是局部,区域和全球大气组合物的重要驱动因子。 2008年OP3项目期间在OP3项目期间的观察结果与一款观察到的箱体模型一起用于评估我们对该氧化化学的理解。符合以前的热带森林的工作,我们发现基于MCM化学的标准模型显着低估了观察到的OH浓度。观察到与异戊二烯影响的OH和HO2的建模比的几何平均分别为5.324.43 + 3.68和1.180.30 + 0.30,其中68%的观察结果在规定的变化范围内。我们实施了各种机械变化进入模型,包括环氧化物形成和异戊二烯过氧自由基的单分子分解,并评估它们对模型成功的影响。我们得出结论,目前的建议都不可以同时消除OH和HO2模拟的偏差,并相信现在需要详细的实验室研究来解决这个问题。
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