ACE-FTS observations of pyrogenic trace species in boreal biomass burning plumes during BORTAS
ACE-FTS observations of pyrogenic trace species in boreal biomass burning plumes during BORTAS
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BORTAS 期间北方生物质燃烧羽流中热解微量物质的 ACE-FTS 观测
DOI：
10.5194/acp-13-4529-2013
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发表时间：
2013
影响因子：
6.3
通讯作者：
P. Bernath
中科院分区：
文献类型：
--
作者：
K. Tereszchuk;G. G. Abad;C. Clerbaux;J. Hadji;D. Hurtmans;P. Coheur;P. Bernath
抽象的。为了进一步了解生物质燃烧排放物对大气成分的影响，2011年7月12日至8月3日在加拿大北方森林火灾季节进行了BORTAS活动（使用飞机和卫星观测大西洋上空对流层氧化剂造成的北方森林火灾）。同时进行的空中、地面和卫星测量活动试图记录北方生物质燃烧的实例，以测量生物质燃烧排放物中短寿命和长寿命痕量分子种类的对流层体积混合比。目的是调查这些热流出物的组成和分布及其对大气化学的干扰之间的联系，特别关注氧化剂种类，以确定对自由对流层氧化能力的总体影响。在BORTAS活动期间，加拿大航天局（加空局）SCISAT-1号卫星上的大气化学实验傅里叶变换光谱仪对北方生物质燃烧羽流中的致热痕量物质进行了测量。尽管生物质燃烧排放物通常局限于边界层，但流出物往往通过孤立的对流和与火灾有关的对流过程注入对流层上部，从而使空间仪器能够测量这些热流出物。分析了CH 3OH、C2 H2、C2 H6、C3 H6 O、CO、HCN、HCOOH、HNO 3、H2 CO、NO、NO2、OCS、O3和PAN等14种分子.包括在这个分析是计算的年龄依赖组的增强比每个物种起源于火灾在北美（加拿大，阿拉斯加）和西伯利亚的一段时间长达7天。寿命较短的主要致热物质的比值随着时间的推移而降低，主要是由于OH自由基的氧化，因为羽状物的年龄和寿命较长的物质，如HCN和C 2 H 6的值保持相对不变。观察到的氧化剂物种，包括O 3，表示销毁过程中的羽流，因为它的年龄，这样的氧化剂物种的浓度已经下降到低于其羽流值的负值。以往的研究结果表明，从测量来自北方火的热质流出物中获得的Δ O3/ΔO摩尔比的值变化很大，范围从负到正，与烟羽年龄无关。这种变异性已被归因于污染的影响，其中的热解流出混合无论是当地的城市氮氧化物排放或热解排放的远程运输的老羽，从而影响生产的O 3羽内。从这项研究的结果已经确定了另一个潜在的原因，在测量生物质燃烧的排放量，平流层对流层交换的证据，由于火灾的热对流上升气流中观察到的O 3浓度的变化。在这些火助对流过程中，由高空排放引起的扰动可能导致平流层空气团侵入自由对流层，随后平流层O3与热源流出物混合，引起观测到的Δ O3/ΔCO摩尔比的波动。
Abstract. To further our understanding of the effects of biomass burning emissions on atmospheric composition, the BORTAS campaign (BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) was conducted on 12 July to 3 August 2011 during the boreal forest fire season in Canada. The simultaneous aerial, ground and satellite measurement campaign sought to record instances of boreal biomass burning to measure the tropospheric volume mixing ratios (VMRs) of short- and long-lived trace molecular species from biomass burning emissions. The goal was to investigate the connection between the composition and the distribution of these pyrogenic outflows and their resulting perturbation to atmospheric chemistry, with particular focus on oxidant species to determine the overall impact on the oxidizing capacity of the free troposphere. Measurements of pyrogenic trace species in boreal biomass burning plumes were made by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) onboard the Canadian Space Agency (CSA) SCISAT-1 satellite during the BORTAS campaign. Even though biomass burning emissions are typically confined to the boundary layer, outflows are often injected into the upper troposphere by isolated convection and fire-related convective processes, thus allowing space-borne instruments to measure these pyrogenic outflows. An extensive set of 14 molecules – CH 3 OH, C 2 H 2 , C 2 H 6 , C 3 H 6 O, CO, HCN, HCOOH, HNO 3 , H 2 CO, NO, NO 2 , OCS, O 3 , and PAN – have been analysed. Included in this analysis is the calculation of age-dependent sets of enhancement ratios for each of the species originating from fires in North America (Canada, Alaska) and Siberia for a period of up to 7 days. Ratio values for the shorter lived primary pyrogenic species decrease over time primarily due to oxidation by the OH radical as the plume ages and values for longer lived species such as HCN and C 2 H 6 remain relatively unchanged. Increasing negative values are observed for the oxidant species, including O 3 , indicating a destruction process in the plume as it ages such that concentrations of the oxidant species have dropped below their off-plume values. Results from previous campaigns have indicated that values for the molar ratios of ΔO 3 /ΔO obtained from the measurements of the pyrogenic outflow from boreal fires are highly variable and range from negative to positive, irrespective of plume age. This variability has been attributed to pollution effects where the pyrogenic outflows have mixed with either local urban NO x emissions or pyrogenic emissions from the long-range transport of older plumes, thus affecting the production of O 3 within the plumes. The results from this study have identified another potential cause of the variability in O 3 concentrations observed in the measurements of biomass burning emissions, where evidence of stratosphere–troposphere exchange due to the pyroconvective updrafts from fires has been identified. Perturbations caused by the lofted emissions in these fire-aided convective processes may result in the intrusion of stratospheric air masses into the free troposphere and subsequent mixing of stratospheric O 3 into the pyrogenic outflows causing fluctuations in observed ΔO 3 /ΔCO molar ratios.
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影响因子：
6.3
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通讯作者：
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影响因子：
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影响因子：
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影响因子：
6.3
作者：
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通讯作者：
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