Ozone photochemistry in boreal biomass burning plumes
Ozone photochemistry in boreal biomass burning plumes
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DOI：
10.5194/acp-13-7321-2013
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发表时间：
2013-08
影响因子：
6.3
通讯作者：
M. Parrington;P. Palmer;A. Lewis;James D. Lee;A. Rickard;P. Carlo;Jonathan P. Taylor;J. Hopkins;S. Punjabi;D. Oram;G. Forster;E. Aruffo;S. Moller;S. Bauguitte;J. Allan;H. Coe;R. Leigh
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文献类型：
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作者：
M. Parrington;P. Palmer;A. Lewis;James D. Lee;A. Rickard;P. Carlo;Jonathan P. Taylor;J. Hopkins;S. Punjabi;D. Oram;G. Forster;E. Aruffo;S. Moller;S. Bauguitte;J. Allan;H. Coe;R. Leigh
抽象。我们提出了一个分析的臭氧（O3）光化学观察到的飞机测量北半球生物质燃烧羽流在加拿大东部在2011年夏天。测量O3和与O3光化学相关的许多关键化学物质，包括非甲烷烃（NMHCs）、氮氧化物（NOx）和总含氮物质（NOy），是由英国FAAM BAe-146研究飞机制造的，作为“使用飞机和卫星量化北方森林火灾对大西洋上空对流层氧化剂的影响”（BORTAS）的一部分。实验于2011年7月12日至8月3日进行。飞机测量的位置和时间使BORTAS处于一个独特的位置，可以对来自安大略西北部同一来源地区的不同年龄的生物质燃烧羽流进行采样。我们发现，在生物质燃烧羽流中测量的O3混合比与非羽流测量结果没有区别，但评估它们与一氧化碳（CO），总烷基硝酸盐（CNOAN）和替代物种NOz（= NOy-NOx）的测量结果的关系显示，O3生产的潜力随羽流年龄的增加。我们使用NMHC比率来估计所观察到的生物质燃烧羽流的光化学年龄在0和10天之间。BORTAS测量提供了采样生物质燃烧羽流中O3产生的宽动态范围，ΔO3/ΔCO增强比从光化学年龄小于2天的羽流中的0.020 ± 0.008 ppbv ppbv−1增加到光化学年龄大于5天的羽流中的0.55 ± 0.29 ppbv ppbv−1。我们发现，在光化学年龄小于4天的烟羽中，ΔO3/ΔCO增强比变化的主要贡献因子是ΔCO，而在光化学年龄大于4天的烟羽中，ΔO3成为主要贡献因子。在比较O3混合比与NOy收支的组成部分时，我们观察到年龄在2到4天之间的羽流的特征是高气溶胶负载，相对湿度大于40%，以及相对于NO2的7.7 ± 3.5 ppbv ppbv−1和相对于NO2的1.6 ± 0.9 ppbv ppbv−1的低臭氧产生效率（OPE）。在大于4天的烟羽中，OPE增加到472 ± 28 ppbv ppbv−1，相对于NOz为155 ± 5 ppbv ppbv−1。从BORTAS的测量，我们估计，低气溶胶负载的老烟羽接近于在光稳态和O3生产在年轻的烟羽被抑制高气溶胶负载和更大的生产相对于O3的O2-AN。BORTAS测量的O3光化学在北方生物质燃烧羽流被认为是一致的，与以前的夏季飞机在同一地区的对流层组成的北极研究（ARCTAS-B）在2008年和大气边界层实验（ABLE 3B）在1990年。
Abstract. We present an analysis of ozone (O3) photochemistry observed by aircraft measurements of boreal biomass burning plumes over eastern Canada in the summer of 2011. Measurements of O3 and a number of key chemical species associated with O3 photochemistry, including non-methane hydrocarbons (NMHCs), nitrogen oxides (NOx) and total nitrogen containing species (NOy), were made from the UK FAAM BAe-146 research aircraft as part of the "quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites" (BORTAS) experiment between 12 July and 3 August 2011. The location and timing of the aircraft measurements put BORTAS into a unique position to sample biomass burning plumes from the same source region in Northwestern Ontario with a range of ages. We found that O3 mixing ratios measured in biomass burning plumes were indistinguishable from non-plume measurements, but evaluating them in relationship to measurements of carbon monoxide (CO), total alkyl nitrates (ΣAN) and the surrogate species NOz (= NOy-NOx) revealed that the potential for O3 production increased with plume age. We used NMHC ratios to estimate photochemical ages of the observed biomass burning plumes between 0 and 10 days. The BORTAS measurements provided a wide dynamic range of O3 production in the sampled biomass burning plumes with ΔO3/ΔCO enhancement ratios increasing from 0.020 ± 0.008 ppbv ppbv−1 in plumes with photochemical ages less than 2 days to 0.55 ± 0.29 ppbv ppbv−1 in plumes with photochemical ages greater than 5 days. We found that the main contributing factor to the variability in the ΔO3/ΔCO enhancement ratio was ΔCO in plumes with photochemical ages less than 4 days, and that was a transition to ΔO3 becoming the main contributing factor in plumes with ages greater than 4 days. In comparing O3 mixing ratios with components of the NOy budget, we observed that plumes with ages between 2 and 4 days were characterised by high aerosol loading, relative humidity greater than 40%, and low ozone production efficiency (OPE) of 7.7 ± 3.5 ppbv ppbv−1 relative to ΣAN and 1.6 ± 0.9 ppbv ppbv−1 relative to NOz. In plumes with ages greater than 4 days, OPE increased to 472 ± 28 ppbv ppbv−1 relative to ΣAN and 155 ± 5 ppbv ppbv−1 relative to NOz. From the BORTAS measurements we estimated that aged plumes with low aerosol loading were close to being in photostationary steady state and O3 production in younger plumes was inhibited by high aerosol loading and greater production of ΣAN relative to O3. The BORTAS measurements of O3 photochemistry in boreal biomass burning plumes were found to be consistent with previous summertime aircraft measurements made over the same region during the Arctic Research of the Composition of the Troposphere (ARCTAS-B) in 2008 and Atmospheric Boundary Layer Experiment (ABLE 3B) in 1990.