DOI: 10.1016/j.atmosenv.2014.03.003
Scopus记录号: 2-s2.0-84896279613
论文题名: Investigating the sensitivity of surface-level nitrate seasonality in Antarctica to primary sources using a global model
作者: Lee H ; -M ; , Henze D ; K ; , Alexander B ; , Murray L ; T
刊名: Atmospheric Environment
ISSN: 0168-2563
EISSN: 1573-515X
出版年: 2014
卷: 89 起始页码: 757
结束页码: 767
语种: 英语
英文关键词: Adjoint based sensitivity analysis
; Antarctica
; GEOS-Chem model
; Total nitrate seasonality
Scopus关键词: Deposition
; Fuels
; Nitrates
; Photolysis
; Soil pollution
; Adjoints
; Antarctica
; Background concentration
; Chemical transport models
; Fossil fuel combustion
; Peroxyacetyl nitrates
; Polar stratospheric clouds
; Seasonality
; Computer simulation
; fossil fuel
; nitrate
; peroxyacetylnitrate
; adjoint method
; atmospheric pollution
; EOS
; global change
; nitrate
; photolysis
; pollutant transport
; sensitivity analysis
; tracer
; altitude
; Antarctica
; article
; cloud
; combustion
; global climate
; lightning
; photolysis
; polar stratospheric cloud
; priority journal
; seasonal variation
; sedimentation
; sensitivity analysis
; stratosphere
; surface property
; troposphere
; winter
; Antarctica
Scopus学科分类: Environmental Science: Water Science and Technology
; Earth and Planetary Sciences: Earth-Surface Processes
; Environmental Science: Environmental Chemistry
英文摘要: Determining the sources of total nitrate (TNIT≡NO3-+HNO3) reaching Antarctica is a long-standing challenge. Here we analyze the monthly sensitivity of surface-level TNIT in Antarctica to primary sources using a global 3-D chemical transport model, GEOS-Chem, and its adjoint. Modeled seasonal variation of TNIT concentrations shows good agreement with several measurement studies, given that the lack of post-depositional processing in the model leads to an expected underestimate of maximum values in November through January. Remote NOx sources have the greatest impact May-July, during when the model background concentrations are sensitive to NOx emissions from fossil fuel combustion, soil, and lightning originating from 25°S to 65°S. In this season, NOx is transported to Antarctica as TNIT, which is formed above continental source regions at an altitude of 5-11km. In other seasons, more NOx is transported as a reservoir species (e.g., peroxyacetyl nitrate, PAN) through the free troposphere, transforming into TNIT within a cone of influence that extends to 35°S and above 4km altitude. Photolysis of PAN over Antarctica is the main driver of modeled NOx seasonality. Stratospheric production and loss of tracers are relatively unimportant in monthly sensitivities in GEOS-Chem, driving only a few percent of surface level variability of TNIT. A small peak concentration in August is captured by the model, although some measured values in August fall outside the range of simulated concentrations. Modifications to the model to represent sedimentation of polar stratospheric clouds (PSCs) lead to increased surface level August TNIT concentrations. However, this simple representation does not explicitly account for PSC particle deposition or disappearance of the tropopause in the middle of winter, and thus the influence of stratospheric nitrate sources estimated in this study is likely a lower bound. © 2014 Elsevier Ltd. Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/80982
Appears in Collections: 气候变化事实与影响
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作者单位: Department of Civil, Environmental and Architectural Engineering, University of Colorado, Boulder, CO 80309, United States; Department of Mechanical Engineering, University of Colorado, Boulder, CO 80309, United States; Department of Atmospheric Sciences, University of Washington, Seattle, WA 98195, United States; School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, United States; Lamont-Doherty Earth Observatory, Columbia University, Palisades, NY 10964, United States
Recommended Citation:
Lee H,-M,, Henze D,et al. Investigating the sensitivity of surface-level nitrate seasonality in Antarctica to primary sources using a global model[J]. Atmospheric Environment,2014-01-01,89