Meyer-Arnek Julian, Ladstätter-Weissenmayer Annette, Richter Andreas, Wittrock Folkard, Burrows John P
Institut für Umweltphysik, Universität Bremen, Otto-Hahn-Allee 2, 28359 Bremen.
Faraday Discuss. 2005;130:387-405; discussion 491-517, 519-24. doi: 10.1039/b502106p.
Retrievals of trace gas columns from the measurements of backscattered radiation by GOME (Global Ozone Monitoring Experiment) show that enhanced tropospheric columns of ozone (O3), nitrogen dioxide (NO2) and formaldehyde (HCHO), over the African continent occur frequently. This study focuses on the behaviour of trace gases over Africa in September 1997, a period impacted by the strongest known El Niño phase of the ENSO. It investigates our qualitative and quantitative understanding of the retrieved tropospheric trace gas column densities. The emissions of NOx and volatile organic compounds (VOC) from biomass burning, biogenic sources and lightning and their photochemical transformation have been investigated. By performing a trajectory analysis, the transport of air masses from the different emission regions was analysed and the potential atmospheric spatial distribution determined. BRemen's Atmospheric PHOtochemical model (BRAPHO) was applied to compute the chemistry along a large number of trajectories. From these results, tropospheric column amounts of O3, NO2 and HCHO were derived. Tropospheric trace gas columns retrieved from GOME measurements and those calculated are in reasonable agreement. Their general spatial extent was similar in the lower troposphere but the modeled trace gas columns in the upper troposphere were located south of the retrieved columns. We attribute this behaviour to uncertainties in the ERA-40 meteorological data in the upper troposphere. The significance of biomass burning and of biogenic emissions with respect to HCHO columns over Africa was investigated. The analysis reveals that the total amounts of HCHO generated over Africa during September 1997 as a result of biomass burning and biogenic emissions are similar. However the HCHO from biogenic sources has the highest specific columns and these are located close to their source. In comparison the HCHO from biomass burning is predicted to be produced and transported over a much wider area. Overall all the emission processes mix together to produce the plume of O3.
通过全球臭氧监测实验(GOME)对后向散射辐射的测量来反演痕量气体柱浓度,结果表明,非洲大陆上空对流层中臭氧(O3)、二氧化氮(NO2)和甲醛(HCHO)柱浓度的增强现象频繁出现。本研究聚焦于1997年9月非洲上空痕量气体的行为,这一时期受到了已知最强厄尔尼诺南方涛动(ENSO)阶段的影响。该研究调查了我们对反演得到的对流层痕量气体柱密度的定性和定量理解。研究了生物质燃烧、生物源和闪电产生的氮氧化物(NOx)和挥发性有机化合物(VOC)排放及其光化学转化过程。通过进行轨迹分析,分析了来自不同排放区域的气团输送情况,并确定了潜在的大气空间分布。应用不来梅大气光化学模型(BRAPHO)来计算沿大量轨迹的化学过程。根据这些结果,得出了对流层中O3、NO2和HCHO的柱含量。从GOME测量中反演得到的对流层痕量气体柱浓度与计算得到的结果吻合较好。它们在对流层下部的总体空间范围相似,但对流层上部模拟得到的痕量气体柱位于反演柱的南侧。我们将这种行为归因于ERA - 40对流层上层气象数据的不确定性。研究了生物质燃烧和生物源排放对非洲上空HCHO柱浓度的重要性。分析表明,1997年9月非洲因生物质燃烧和生物源排放产生的HCHO总量相似。然而,生物源产生的HCHO具有最高的比柱浓度,且这些HCHO位于靠近其源的位置。相比之下,预计生物质燃烧产生的HCHO会在更广泛的区域产生和输送。总体而言,所有排放过程混合在一起形成了O3羽流。