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Quantification of the unknown HONO daytime source and its relation to NO_2

机译:未知HONO日源的量化及其与NO_2的关系

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During the DOMINO (Diel Oxidant Mechanism In relation to Nitrogen Oxides) campaign in southwest Spain we measured simultaneously all quantities necessary to calculate a photostationary state for HONO in the gas phase. These quantities comprise the concentrations of OH, NO, and HONO and the photolysis frequency of NO_2, j(NO_2) as a proxy for j(HONO). This allowed us to calculate values of the unknown HONO daytime source. This unknown HONO source, normalized by NO_2 mixing ratios and expressed as a conversion frequency (% h~(-1)), showed a clear dependence on j(NO_2) with values up to 43% h~(-1) at noon. We compared our unknown HONO source with values calculated from the measured field data for two recently proposed processes, the light-induced NO_2 conversion on soot surfaces and the reaction of electronically excited NO_2~* with water vapour, with the result that these two reactions normally contributed less than 10% (<1% NO_2 + soot + hν and <10% NO_2~* + H_2O) to our unknown HONO daytime source. OH production from HONO photolysis was found to be larger (by 20%) than the "classical" OH formation from ozone photolysis (O(1D)) integrated over the day.
机译:在西班牙西南部的DOMINO(与氮氧化物相关的狄尔氧化剂机理)研究活动中,我们同时测量了计算气相中HONO的光固定态所需的所有量。这些量包括OH,NO和HONO的浓度以及NO_2,j(NO_2)的光解频率,以替代j(HONO)。这使我们能够计算未知的HONO白天源的值。该未知的HONO源通过NO_2混合比归一化并表示为转化频率(%h〜(-1)),显示出对j(NO_2)的明显依赖性,中午时值高达h%(-1)达43%。我们将未知的HONO源与根据最近提出的两个过程(实测烟灰表面上的光诱导NO_2转化以及电子激发的NO_2〜*与水蒸气的反应)的实测数据计算得出的值进行比较,结果这两个反应正常对我们未知的HONO日间源的贡献少于10%(<1%NO_2 +烟灰+hν和<10%NO_2〜* + H_2O)。发现一天中从HONO光解产生的OH数量要大(增加20%),比从臭氧光解(O(1D))产生的“经典” OH生成量大。

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