Multi-model study of chemical and physical controls on transport of anthropogenic and biomass burning pollution to the Arctic-猫眼课题宝

DOI：

10.5194/acp-15-3575-2015

发表时间：

2014-10

期刊：

Atmospheric Chemistry and Physics

影响因子：

6.3

通讯作者：

中科院分区：

地球科学1区

文献类型：

作者：

S. Monks;S. Monks;S. Monks;S. Arnold;L. Emmons;K. Law;S. Turquety;B. Duncan;J. Flemming;V. Huijnen;S. Tilmes;J. Langner;J. Mao;Y. Long;Jennie L. Thomas;S. Steenrod;Jean-Christophe Raut;Chris Wilson;M. Chipperfield;G. Diskin;A. Weinheimer;H. Schlager;G. Ancellet

利用飞机，地面站和卫星的观测，我们全面评估多模式模拟一氧化碳（CO）和臭氧（O3）在北极和低纬度排放地区，作为POLARCAT模型相互比较项目（POLMIP）的一部分。11个大气模型与化学的评估表明，他们普遍低估了整个北极对流层的CO，在冬季和春季发现的最大偏差。在整个北方半球也发现了负CO偏差，多模型平均粗差（9-12%）表明模型在亚洲、北美和欧洲的表现相似。多模式年平均对流层OH（10.8 ± 0.6 × 105 molec cm−3）被发现略高于以前的估计的OH限制甲基氯仿，这表明模式中的负CO偏差可能会通过更好的限制OH得到改善。具有较低的北极OH的模型并不总是表现出显着的改善，在他们的负CO偏差，这表明北极OH是不是在这些模型中控制北极CO负担的主导因素。除了这些一般的偏差，模型不捕捉在北极自由对流层在夏季观察到的CO增强的幅度，这表明在模拟从低纬度的人为和生物质燃烧源输送的羽流的模型误差。北极的O3也普遍被低估，特别是在地表和对流层上部。夏季O3在低纬度地区的比较表明，几个模型高估了对流层上层的浓度。模拟的CO、O3和OH都表现出相当程度的模型间变异性。理想化的CO样示踪剂被用来定量比较模型间的运输和OH CO在北极对流层的差异的影响。示踪剂表明，从欧洲在冬季和亚洲全年的模式差异运输模式变异的重要来源，在巴罗。与运输不同，OH的模型间变异同样影响巴罗的所有区域示踪剂。固定的寿命和OH损失理想化的CO示踪剂在整个北极对流层的比较表明，OH的差异是一个更大的源模型间的变异性比运输的差异。模型中的OH浓度与模型间的H2O差异相关，这表明它是这些模拟中高纬度CO和OH模拟浓度差异的重要驱动因素。尽管模型间在传输和OH方面存在差异，但不同来源区域（北美、欧洲和亚洲）和不同来源类型（人为和生物量燃烧）的相对贡献在模型间是可比的。在2008年从北方地区的火灾排放贡献33%，43%和19%的北极类CO示踪剂在春季，夏季和秋季，分别突出了北方火灾排放在控制污染物的负担在北极的重要性。

Using observations from aircraft, surface stations and satellite, we comprehensively evaluate multi-model simulations of carbon monoxide (CO) and ozone (O3) in the Arctic and over lower latitude emission regions, as part of the POLARCAT Model Inter-comparison Project (POLMIP). Evaluation of eleven atmospheric models with chemistry shows that they generally underestimate CO throughout the Arctic troposphere, with the largest biases found during winter and spring. Negative CO biases are also found throughout the Northern Hemisphere, with multi-model mean gross errors (9-12%) suggesting models perform similarly over Asia, North America and Europe. A multi-model annual mean tropospheric OH (10.8 ± 0.6 × 105 molec cm−3) is found to be slightly higher than previous estimates of OH constrained by methyl chloroform, suggesting negative CO biases in models may be improved through better constraints on OH. Models that have lower Arctic OH do not always show a substantial improvement in their negative CO biases, suggesting that Arctic OH is not the dominant factor controlling the Arctic CO burden in these models. In addition to these general biases, models do not capture the magnitude of CO enhancements observed in the Arctic free troposphere in summer, suggesting model errors in the simulation of plumes that are transported from anthropogenic and biomass burning sources at lower latitudes. O3 in the Arctic is also generally underestimated, particularly at the surface and in the upper troposphere. Summer O3 comparisons over lower latitudes show several models overestimate upper tropospheric concentrations. Simulated CO, O3 and OH all demonstrate a substantial degree of inter-model variability. Idealised CO-like tracers are used to quantitatively compare the impact of inter-model differences in transport and OH on CO in the Arctic troposphere. The tracers show that model differences in transport from Europe in winter and from Asia throughout the year are important sources of model variability at the Barrow. Unlike transport, inter-model variability in OH similarly affects all regional tracers at Barrow. Comparisons of fixed lifetime and OH-loss idealised CO-like tracers throughout the Arctic troposphere show that OH differences are a much larger source of inter-model variability than transport differences. The concentration of OH in the models is found to be correlated with inter-model differences in H2O, suggesting it to be an important driver of differences in simulated concentrations of CO and OH at high latitudes in these simulations. Despite inter-model differences in transport and OH, the relative contributions from the different source regions (North America, Europe and Asia) and different source types (anthropogenic and biomass burning) are comparable across the models. Fire emissions from the boreal regions in 2008 contribute 33, 43 and 19% to the total Arctic CO-like tracer in spring, summer and autumn, respectively, highlighting the importance of boreal fire emissions in controlling pollutant burdens in the Arctic.

Multi-model study of chemical and physical controls on transport of anthropogenic and biomass burning pollution to the Arctic

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