Photochemical production of ozone in the upper troposphere in association with cumulus convection over Indonesia

Photochemical production of ozone in the upper troposphere in association with cumulus convection over Indonesia
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DOI:
10.1029/2001jd000844
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发表时间:
2002-02
影响因子:
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通讯作者:
K. Kita;S. Kawakami;Y. Miyazaki;Y. Higashi;Y. Kondo;N. Nishi;M. Koike;D. Blake;T. Machida;T. Sano;Weiwei Hu;M. Ko;T. Ogawa
K. Kita;S. Kawakami;Y. Miyazaki;Y. Higashi;Y. Kondo;N. Nishi;M. Koike;D. Blake;T. Machida;T. Sano;Weiwei Hu;M. Ko;T. Ogawa
中科院分区:
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文献类型:
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作者:
K. Kita;S. Kawakami;Y. Miyazaki;Y. Higashi;Y. Kondo;N. Nishi;M. Koike;D. Blake;T. Machida;T. Sano;Weiwei Hu;M. Ko;T. Ogawa

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[1]1998年9月24日至10月10日在拉尼娜期间进行了生物量燃烧和闪电实验A阶段(BIBLE-A)飞机观测活动。在这场运动中,臭氧及其前体(NO,CO和非甲烷烃(NMHCs))的分布在热带太平洋,印度尼西亚和澳大利亚北方。在热带太平洋上空0 - 13.5公里高度处,臭氧及其前体物的混合比很低。印度尼西亚上空8公里以上的臭氧前体物的混合比通常明显高于热带太平洋上空的混合比,尽管盛行的东风在几天内将热带太平洋的空气带到印度尼西亚上空。例如,对流层上层的NO和CO混合比中值在热带太平洋上为万亿分之12(pptv)和十亿分之72(ppbv),在印度尼西亚西部分别为83 pptv和85 ppbv。气象分析和高乙烯(C2 H4)的混合比表明,增加的臭氧前体物是由活跃的对流在印度尼西亚通过向上输送的污染空气,混合,和闪电都在几天内观察前。通过比较对流层低层和高层NMHCs和CH 3Cl浓度与CO的相关性,讨论了臭氧前体物的来源。在IBLE-A期间,印度尼西亚的生物质燃烧几乎不活跃,并不是臭氧前体物的主要来源,但城市污染和闪电对它们的增加起到了重要作用。如光化学模式计算所示,臭氧前体物的增加提高了印度尼西亚西部对流层上层的臭氧净生成率。然而,印度尼西亚上空的臭氧混合比(20 ppbv)并未显著增加,因为臭氧的光化学生成自臭氧前体增加以来没有足够的时间。反向轨迹显示,在印度尼西亚南部海洋和澳大利亚北方上空采样的许多气团在测量前4-9天经过印度尼西亚西部。在这些空气质量的臭氧前体物的混合比,除了短寿命的物种,是类似的印度尼西亚西部。与此相反,臭氧混合比比印度尼西亚上空高出约10 ppbv,表明臭氧的光化学产生发生在印度尼西亚的输送过程中。在这种传输过程中,臭氧的平均增长率(1.8 ppbv/d)与光化学模型计算的臭氧净形成率相似。这项研究表明,活跃的对流在印度尼西亚进行污染空气从地面向上,并有明显的影响,在对流层上部的臭氧分布在印度洋,澳大利亚北方,南亚热带太平洋,结合NO生产闪电。
[1] The Biomass Burning and Lightning Experiment phase A (BIBLE-A) aircraft observation campaign was conducted from 24 September to 10 October 1998, during a La Nina period. During this campaign, distributions of ozone and its precursors (NO, CO, and nonmethane hydrocarbons (NMHCs)) were observed over the tropical Pacific Ocean, Indonesia, and northern Australia. Mixing ratios of ozone and its precursors were very low at altitudes between 0 and 13.5 km over the tropical Pacific Ocean. The mixing ratios of ozone precursors above 8 km over Indonesia were often significantly higher than those over the tropical Pacific Ocean, even though the prevailing easterlies carried the air from the tropical Pacific Ocean to over Indonesia within several days. For example, median NO and CO mixing ratios in the upper troposphere were 12 parts per trillion (pptv) and 72 parts per billion (ppbv) over the tropical Pacific Ocean and were 83 pptv and 85 ppbv over western Indonesia, respectively. Meteorological analyses and high ethene (C2H4) mixing ratios indicate that the increase of the ozone precursors was caused by active convection over Indonesia through upward transport of polluted air, mixing, and lightning all within the few days prior to observation. Sources of ozone precursors are discussed by comparing correlations of some NMHCs and CH3Cl concentrations with CO between the lower and upper troposphere. Biomass burning in Indonesia was nearly inactive during BIBLE-A and was not a dominant source of the ozone precursors, but urban pollution and lightning contributed importantly to their increases. The increase in ozone precursors raised net ozone production rates over western Indonesia in the upper troposphere, as shown by a photochemical model calculation. However, the ozone mixing ratio (∼20 ppbv) did not increase significantly over Indonesia because photochemical production of ozone did not have sufficient time since the augmentation of ozone precursors. Backward trajectories show that many air masses sampled over the ocean south of Indonesia and over northern Australia passed over western Indonesia 4–9 days prior to being measured. In these air masses the mixing ratios of ozone precursors, except for short-lived species, were similar to those over western Indonesia. In contrast, the ozone mixing ratio was higher by about 10 ppbv than that over Indonesia, indicating that photochemical production of ozone occurred during transport from Indonesia. The average rate of ozone increase (1.8 ppbv/d) during this transport is similar to the net ozone formation rate calculated by the photochemical model. This study shows that active convection over Indonesia carried polluted air upward from the surface and had a discernable influence on the distribution of ozone in the upper troposphere over the Indian Ocean, northern Australia, and the south subtropical Pacific Ocean, combined with NO production by lightning.