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首页> 外文期刊>Atmospheric Chemistry and Physics Discussions >Reactive nitrogen, ozone and ozone production in the Arctic troposphere and the impact of stratosphere-troposphere exchange
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Reactive nitrogen, ozone and ozone production in the Arctic troposphere and the impact of stratosphere-troposphere exchange

机译:反应性氮,臭氧和臭氧生产在北极对流层和平流层 - 对流层交换的影响

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We use aircraft observations obtained during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission to examine the distributions and source attributions of O3 and NOy in the Arctic and sub-Arctic region. Using a number of marker tracers, we distinguish various air masses from the background troposphere and examine their contributions to NOx, O3, and O3 production in the Arctic troposphere. The background Arctic troposphere has a mean O3 of ~60 ppbv and NOx of ~25 pptv throughout spring and summer with CO decreasing from ~145 ppbv in spring to ~100 ppbv in summer. These observed mixing ratios are not notably different from the values measured during the 1988 ABLE-3A and the 2002 TOPSE field campaigns despite the significant changes in emissions and stratospheric ozone layer in the past two decades that influence Arctic tropospheric composition. Air masses associated with stratosphere-troposphere exchange are present throughout the mid and upper troposphere during spring and summer. These air masses, with mean O3 concentrations of 140–160 ppbv, are significant direct sources of O3 in the Arctic troposphere. In addition, air of stratospheric origin displays net O3 formation in the Arctic due to its sustainable, high NOx (75 pptv in spring and 110 pptv in summer) and NOy (~800 pptv in spring and ~1100 pptv in summer). The air masses influenced by the stratosphere sampled during ARCTAS-B also show conversion of HNO3 to PAN. This active production of PAN is the result of increased degradation of ethane in the stratosphere-troposphere mixed air mass to form CH3CHO, followed by subsequent formation of PAN under high NOx conditions. These findings imply that an adequate representation of stratospheric NOy input, in addition to stratospheric O3 influx, is essential to accurately simulate tropospheric Arctic O3, NOx and PAN in chemistry transport models. Plumes influenced by recent anthropogenic and biomass burning emissions observed during ARCTAS show highly elevated levels of hydrocarbons and NOy (mostly in the form of NOx and PAN), but do not contain O3 higher than that in the Arctic tropospheric background except some aged biomass burning plumes sampled during spring. Convection and/or lightning influences are negligible sources of O3 in the Arctic troposphere but can have significant impacts in the upper troposphere in the continental sub-Arctic during summer.
机译:我们使用飞机观察在飞机和卫星(ARCTAS)任务的对流层组成的北极研究期间获得的,以检查北极和亚北极地区O3和NOY的分布和源归因。使用许多标记示踪剂,我们将各种空气群体区分离出背景对流层,并在北极对流层中考虑对NOx,O3和O3生产的贡献。背景北极对流层在夏季和夏季的春季和夏季〜25 pptv的平均o3〜25 pptv的〜25 pptv,夏季春季〜100 ppbv〜145 ppbv。这些观察到的混合比率与在1988年的能够 - 3A和2002个上部野外活动期间测量的值不具有显着不同,尽管过去二十年来减少排放和平流层臭氧层的显着变化,但影响了北极对流层组成。与平流层 - 对流层交流相关的空气群众在春季和夏季期间在整个半层和上层。这些空气质量为140-160ppbv的平均O 3浓度,是北极对流层中O3的显着直接来源。此外,平流层的空气由于其可持续,高Nox(夏季春季和110 pptv,春季110 pptv,春季〜1100 pptv〜1100 pptv,夏季春季和〜1100 pptv,在北极而在北极形成净O3形成。受Arctas-B期间采样的平流层影响的空气群体也显示出HNO3转化为PAN。该PAN的活性生产是在平流层 - 对流层混合空气质量中增加乙烷的降解,以形成CH3芯片,然后在高NOx条件下形成锅。这些发现暗示,除了平流层O3流入之外,平流层NOY输入的足够表示对于精确地模拟化学输送模型中的对流层北极O3,NOx和PAN至关重要。在ARCTAS期间观察到最近的人类学和生物质燃烧排放的羽毛显示出高度升高的碳氢化合物和NOY(主要以NOx和PAN的形式),但不含有高于北极对流层背景的O3,除了一些老化的生物量燃烧羽毛在春天抽样。对流和/或避雷的影响是北极对流层中O3的可忽略的来源,但在夏季,欧洲北极北极的上层对流层中的较高影响可能会产生重大影响。
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