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DOI | 10.1029/2019GL081990 |
The Role of Clouds in the Tropospheeric NOx Cycle: A New Modeling Approach for Cloud Chemistry and Its Global Implications | |
Holmes, Christopher D.1; Bertram, Timothy H.2; Confer, Kaitlyn L.1; Grahams, Kelly A.1; Ronan, Allison C.1; Wirks, Charles K.1; Shah, Viral3 | |
2019-05-16 | |
发表期刊 | GEOPHYSICAL RESEARCH LETTERS
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ISSN | 0094-8276 |
EISSN | 1944-8007 |
出版年 | 2019 |
卷号 | 46期号:9页码:4980-4990 |
文章类型 | Article |
语种 | 英语 |
国家 | USA |
英文摘要 | We present a new method for simulating heterogeneous (surface and multiphase) cloud chemistry in atmospheric models that do not spatially resolve clouds. The method accounts for cloud entrainment within the chemical rate expression, making it more accurate and stable than other approaches. Using this "entrainment-limited uptake," we evaluate the role of clouds in the tropospheric NOx cycle. Past literature suggests that on large scales, losses of N2O5 and NO3 in clouds are much less important than losses on aerosols. We find, however, that cloud reactions provide 25% of tropospheric NOx loss in high latitudes and 5% of global loss. Homogeneous, gas phase hydrolysis of N2O5 is likely 2% or less of global NO, loss. Both clouds and aerosols have similar impacts on global tropospheric O-3 and OH levels, around 2% each. Accounting for cloud uptake reduces the sensitivity of atmospheric chemistry to aerosol surface area and uptake coefficient since clouds and aerosols compete for the same NO3 and N2O5. Plain Language Summary Cloud water droplets and ice crystals enable some aqueous and surface chemical reactions that otherwise would not occur in the gaseous atmosphere. While clouds are widespread and familiar, methods for simulating their multiphase chemical effects in global atmospheric models have been inadequate. We present an efficient mathematical method to represent the combined effects of cloud chemistry and entrainment in large-scale atmospheric chemistry models that do not resolve individual clouds. By applying the approach to nitrogen oxides, we show that clouds have a previously unrecognized impact on tropospheric ozone, an air pollutant and greenhouse gas, and hydroxyl, a key atmospheric oxidant. |
领域 | 气候变化 |
收录类别 | SCI-E |
WOS记录号 | WOS:000468869500047 |
WOS关键词 | GENERAL-CIRCULATION MODEL ; SECONDARY ORGANIC AEROSOL ; ATMOSPHERIC CHEMISTRY ; HETEROGENEOUS REACTIONS ; NITROGEN-OXIDES ; PHOTOCHEMICAL DATA ; GASEOUS N2O5 ; EMISSIONS ; OZONE ; CLIMATE |
WOS类目 | Geosciences, Multidisciplinary |
WOS研究方向 | Geology |
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/183283 |
专题 | 气候变化 |
作者单位 | 1.Florida State Univ, Dept Earth Ocean & Atmospher Sci, Tallahassee, FL 32306 USA; 2.Univ Wisconsin, Dept Chem, 1101 Univ Ave, Madison, WI 53706 USA; 3.Harvard Univ, Harvard A John Paulson Sch Engn & Appl Sci, Cambridge, MA 02138 USA |
推荐引用方式 GB/T 7714 | Holmes, Christopher D.,Bertram, Timothy H.,Confer, Kaitlyn L.,et al. The Role of Clouds in the Tropospheeric NOx Cycle: A New Modeling Approach for Cloud Chemistry and Its Global Implications[J]. GEOPHYSICAL RESEARCH LETTERS,2019,46(9):4980-4990. |
APA | Holmes, Christopher D..,Bertram, Timothy H..,Confer, Kaitlyn L..,Grahams, Kelly A..,Ronan, Allison C..,...&Shah, Viral.(2019).The Role of Clouds in the Tropospheeric NOx Cycle: A New Modeling Approach for Cloud Chemistry and Its Global Implications.GEOPHYSICAL RESEARCH LETTERS,46(9),4980-4990. |
MLA | Holmes, Christopher D.,et al."The Role of Clouds in the Tropospheeric NOx Cycle: A New Modeling Approach for Cloud Chemistry and Its Global Implications".GEOPHYSICAL RESEARCH LETTERS 46.9(2019):4980-4990. |
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