GSTDTAP  > 地球科学
DOI10.5194/acp-19-12091-2019
Nonlinear behavior of organic aerosol in biomass burning plumes: a microphysical model analysis
Konovalov, Igor B.1; Beekmann, Matthias2; Goloyushkin, Nikolai A.1; Andreae, Meinrat O.3,4,5
2019-09-30
发表期刊ATMOSPHERIC CHEMISTRY AND PHYSICS
ISSN1680-7316
EISSN1680-7324
出版年2019
卷号19期号:19页码:12091-12119
文章类型Article
语种英语
国家Russia; France; Germany; USA; Saudi Arabia
英文摘要

Organic aerosol (OA) is a major component of smoke plumes from open biomass burning (BB). Therefore, adequate representation of the atmospheric transformations of BB OA in chemistry-transport and climate models is an important prerequisite for accurate estimates of the impact of BB emissions on air quality and climate. However, field and laboratory studies of atmospheric transformations (aging) of BB OA have yielded a wide diversity of observed effects. This diversity is still not sufficiently understood and thus not addressed in models. As OA evolution is governed by complex nonlinear processes, it is likely that at least a part of the observed variability in the BB OA aging effects is due to the factors associated with the intrinsic nonlinearity of the OA system. In this study, we performed a numerical analysis in order to gain a deeper understanding of these factors. We employ a microphysical dynamic model that represents gas particle partitioning and OA oxidation chemistry within the volatility basis set (VBS) framework and includes a schematic parameterization of BB OA dilution due to dispersion of an isolated smoke plume. Several VBS schemes of different complexity, which have been suggested in the literature to represent BB OA aging in regional and global chemistry-transport models, are applied to simulate BB OA evolution over a 5 d period representative of the BB aerosol lifetime in the dry atmosphere. We consider the BB OA mass enhancement ratio (EnR), which is defined as the ratio of the mass concentration of BB OA to that of an inert tracer and allows us to eliminate the linear part of the dilution effects. We also analyze the behavior of the hygroscopicity parameter, that was simulated in a part of our numerical experiments. As a result, five qualitatively different regimes of OA evolution are identified, which comprise (1) a monotonic saturating increase in EnR, (2) an increase in EnR followed by a decrease, (3) an initial rapid decrease in EnR followed by a gradual increase, (4) an EnR increase between two intermittent stages of its decrease, or (5) a gradual decrease in EnR. We find that the EnR for BB aerosol aged from a few hours to a few tens of hours typically increases for larger initial sizes of the smoke plume (and therefore smaller dilution rates) or for lower initial OA concentrations (and thus more organic gases available to form secondary OA - SOA). However, these dependencies can be weakened or even reversed, depending on the BB OA age and on the ratio between the fragmentation and functionalization oxidation pathways. Nonlinear behavior of BB OA is also exhibited in the dependencies of kappa on the parameters of the plume. Application of the different VBS schemes results in large quantitative and qualitative differences between the simulations, although our analysis suggests also that the main qualitative features of OA evolution simulated with a complex two-dimensional VBS scheme can also be reproduced with a much simpler scheme. Overall, this study indicates that the BB aerosol evolution may strongly depend on parameters of the individual BB smoke plumes (such as the initial organic aerosol concentration and plume size) that are typically not resolved in chemistry-transport models.


领域地球科学
收录类别SCI-E
WOS记录号WOS:000488976600002
WOS关键词VOLATILITY BASIS-SET ; TOWER OBSERVATORY ZOTTO ; BROWN CARBON ; BLACK CARBON ; SATELLITE-OBSERVATIONS ; CHEMICAL-COMPOSITION ; MEXICO-CITY ; TRACE GASES ; EMISSIONS ; EVOLUTION
WOS类目Environmental Sciences ; Meteorology & Atmospheric Sciences
WOS研究方向Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
引用统计
文献类型期刊论文
条目标识符http://119.78.100.173/C666/handle/2XK7JSWQ/187151
专题地球科学
作者单位1.Russian Acad Sci, Inst Appl Phys, Nizhnii Novgorod, Russia;
2.Univ Paris, Univ Paris Est Creteil, UMR 7583, Inst Pierre Simon Laplace,LISA,CNRS, Creteil, France;
3.Max Planck Inst Chem, Mainz, Germany;
4.Univ Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA;
5.King Saud Univ, Dept Geol & Geophys, Riyadh, Saudi Arabia
推荐引用方式
GB/T 7714
Konovalov, Igor B.,Beekmann, Matthias,Goloyushkin, Nikolai A.,et al. Nonlinear behavior of organic aerosol in biomass burning plumes: a microphysical model analysis[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2019,19(19):12091-12119.
APA Konovalov, Igor B.,Beekmann, Matthias,Goloyushkin, Nikolai A.,&Andreae, Meinrat O..(2019).Nonlinear behavior of organic aerosol in biomass burning plumes: a microphysical model analysis.ATMOSPHERIC CHEMISTRY AND PHYSICS,19(19),12091-12119.
MLA Konovalov, Igor B.,et al."Nonlinear behavior of organic aerosol in biomass burning plumes: a microphysical model analysis".ATMOSPHERIC CHEMISTRY AND PHYSICS 19.19(2019):12091-12119.
条目包含的文件
条目无相关文件。
个性服务
推荐该条目
保存到收藏夹
查看访问统计
导出为Endnote文件
谷歌学术
谷歌学术中相似的文章
[Konovalov, Igor B.]的文章
[Beekmann, Matthias]的文章
[Goloyushkin, Nikolai A.]的文章
百度学术
百度学术中相似的文章
[Konovalov, Igor B.]的文章
[Beekmann, Matthias]的文章
[Goloyushkin, Nikolai A.]的文章
必应学术
必应学术中相似的文章
[Konovalov, Igor B.]的文章
[Beekmann, Matthias]的文章
[Goloyushkin, Nikolai A.]的文章
相关权益政策
暂无数据
收藏/分享
所有评论 (0)
暂无评论
 

除非特别说明,本系统中所有内容都受版权保护,并保留所有权利。