Analysis of ozone and nitric acid in spring and summer Arctic pollution using aircraft, ground-based, satellite observations and MOZART-4 model: source attribution and partitioning

Analysis of ozone and nitric acid in spring and summer Arctic pollution using aircraft, ground-based, satellite observations and MOZART-4 model: source attribution and partitioning
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利用飞机、地面、卫星观测和 MOZART-4 模型分析春季和夏季的臭氧和硝酸北极污染:来源归因和分区

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发表时间:
2011
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通讯作者:
P. Wennberg
P. Wennberg
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作者:
C. Wespes;L. Emmons;D. Edwards;J. Hannigan;D. Hurtmans;M. Saunois;P. Coheur;C. Clerbaux;M. Coffey;R. Batchelor;R. Lindenmaier;K. Strong;A. Weinheimer;J. Nowak;T. Ryerson;J. Crounse;P. Wennberg

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抽象的。在本文中,我们在 POLARCAT(使用飞机、遥感、气候、化学、气溶胶和运输的表面测量和模型进行极地研究)计划期间结合观测结果和模型结果分析了对流层 O 3 和 HNO 3 。 2008 年春季和夏季期间,NASA ARCTAS(飞机和卫星对流层组成的北极研究)和 NOAA ARCPAC(影响北极气候的气溶胶、辐射和云过程)活动的飞机观测与臭氧和相关化学示踪剂模型第 4 版 (MOZART-4) 一起使用,以协助解释 O 3 和 HNO 3 的来源归属以及向北极的迁移方面的观测结果(北纬 60°以北)。 MOZART-4 模拟总体上很好地再现了飞机观测结果(误差在 15% 以内),但模型中的一些差异也得到了识别和讨论。利用观察到的 O 3 与 HNO 3 的相关性来评估不同气团类型(新鲜羽流、自由对流层和平流层污染气团)的 MOZART-4 模型性能。基于按来源类型和区域标记的O 3 和HNO 3 模型模拟,我们发现北半球的人为污染是北极地区压力大于400 hPa时O 3 和HNO 3 的主要来源,而压力小于400 hPa时平流层的影响是主要贡献。夏季,俄罗斯强烈的火排放对美国北极地区上空的对流层中的两种气体产生了一定程度的影响。北美火灾排放物(加利福尼亚和加拿大)也对北极边界层的对流层臭氧产生重要影响。使用标记的贡献对 POLARCAT 期间在尤里卡(加拿大)和图勒(格陵兰)极地站点进行的地面 FTIR 和 IASI 卫星探测仪进行的对流层 O 3 测量进行了附加分析。它展示了这些仪器观测北部高纬度地区污染的能力。通过 FTIR 和 IASI 测量的源对对流层柱的贡献之间的差异根据与这些仪器相关的垂直灵敏度进行了讨论。还提供了 IASI 卫星仪器在北极观测到的 O 3 对流层柱的首次分析。尽管 IASI 在最低大气层的垂直灵敏度有限,但我们证明 IASI 能够检测输送到北极的低空污染,但存在一些局限性。
Abstract. In this paper, we analyze tropospheric O 3 together with HNO 3 during the POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols, and Transport) program, combining observations and model results. Aircraft observations from the NASA ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) and NOAA ARCPAC (Aerosol, Radiation and Cloud Processes affecting Arctic Climate) campaigns during spring and summer of 2008 are used together with the Model for Ozone and Related Chemical Tracers, version 4 (MOZART-4) to assist in the interpretation of the observations in terms of the source attribution and transport of O 3 and HNO 3 into the Arctic (north of 60° N). The MOZART-4 simulations reproduce the aircraft observations generally well (within 15%), but some discrepancies in the model are identified and discussed. The observed correlation of O 3 with HNO 3 is exploited to evaluate the MOZART-4 model performance for different air mass types (fresh plumes, free troposphere and stratospheric-contaminated air masses). Based on model simulations of O 3 and HNO 3 tagged by source type and region, we find that the anthropogenic pollution from the Northern Hemisphere is the dominant source of O 3 and HNO 3 in the Arctic at pressures greater than 400 hPa, and that the stratospheric influence is the principal contribution at pressures less 400 hPa. During the summer, intense Russian fire emissions contribute some amount to the tropospheric columns of both gases over the American sector of the Arctic. North American fire emissions (California and Canada) also show an important impact on tropospheric ozone in the Arctic boundary layer. Additional analysis of tropospheric O 3 measurements from ground-based FTIR and from the IASI satellite sounder made at the Eureka (Canada) and Thule (Greenland) polar sites during POLARCAT has been performed using the tagged contributions. It demonstrates the capability of these instruments for observing pollution at northern high latitudes. Differences between contributions from the sources to the tropospheric columns as measured by FTIR and IASI are discussed in terms of vertical sensitivity associated with these instruments. The first analysis of O 3 tropospheric columns observed by the IASI satellite instrument over the Arctic is also provided. Despite its limited vertical sensitivity in the lowermost atmospheric layers, we demonstrate that IASI is capable of detecting low-altitude pollution transported into the Arctic with some limitations.