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DOI10.5194/acp-22-4253-2022
Photochemical evolution of the 2013 California Rim Fire: synergistic impacts of reactive hydrocarbons and enhanced oxidants
Wolfe, Glenn M.; Hanisco, Thomas F.; Arkinson, Heather L.; Blake, Donald R.; Wisthaler, Armin; Mikoviny, Tomas; Ryerson, Thomas B.; Pollack, Ilana; Peischl, Jeff; Wennberg, Paul O.; Crounse, John D.; St. Clair, Jason M.; Teng, Alex; Huey, L. Gregory; Liu, Xiaoxi; Fried, Alan; Weibring, Petter; Richter, Dirk; Walega, James; Hall, Samuel R.; Ullmann, Kirk; Jimenez, Jose L.; Campuzano-Jost, Pedro; Bui, T. Paul; Diskin, Glenn; Podolske, James R.; Sachse, Glen; Cohen, Ronald C.
发表日期2022
ISSN1680-7316
EISSN1680-7324
起始页码4253
结束页码4275
卷号22期号:6页码:23
英文摘要Large wildfires influence regional atmospheric composition, but chemical complexity challenges model predictions of downwind impacts. Here, we elucidate key connections within gas-phase photochemistry and assess novel chemical processes via a case study of the 2013 California Rim Fire plume. Airborne in situ observations, acquired during the NASA Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC(4)RS) mission, illustrate the evolution of volatile organic compounds (VOCs), oxidants, and reactive nitrogen over 12 h of atmospheric aging. Measurements show rapid formation of ozone and peroxyacyl nitrates (PNs), sustained peroxide production, and prolonged enhancements in oxygenated VOCs and nitrogen oxides (NOx). Observations and Lagrangian trajectories constrain a 0-D puff model that approximates plume photochemical history and provides a framework for evaluating process interactions. Simulations examine the effects of (1) previously unmeasured reactive VOCs identified in recent laboratory studies and (2) emissions and secondary production of nitrous acid (HONO). Inclusion of estimated unmeasured VOCs leads to a 250 % increase in OH reactivity and a 70 % increase in radical production via oxygenated VOC photolysis. HONO amplifies radical cycling and serves as a downwind NOx source, although impacts depend on how HONO is introduced. The addition of initial HONO (representing primary emissions) or particulate nitrate photolysis amplifies ozone production, while heterogeneous conversion of NO2 suppresses ozone formation. Analysis of radical initiation rates suggests that oxygenated VOC photolysis is a major radical source, exceeding HONO photolysis when averaged over the first 2 h of aging. Ozone production chemistry transitions from VOC sensitive to NOx sensitive within the first hour of plume aging, with both peroxide and organic nitrate formation contributing significantly to radical termination. To simulate smoke plume chemistry accurately, models should simultaneously account for the full reactive VOC pool and all relevant oxidant sources.
学科领域Environmental Sciences; Meteorology & Atmospheric Sciences
语种英语
WOS研究方向Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
WOS记录号WOS:000776667600001
来源期刊ATMOSPHERIC CHEMISTRY AND PHYSICS
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/273500
作者单位National Aeronautics & Space Administration (NASA); NASA Goddard Space Flight Center; University System of Maryland; University of Maryland College Park; University of California System; University of California Irvine; University of Innsbruck; University of Oslo; National Oceanic Atmospheric Admin (NOAA) - USA; University of Colorado System; University of Colorado Boulder; California Institute of Technology; California Institute of Technology; University System of Georgia; Georgia Institute of Technology; University of Colorado System; University of Colorado Boulder; National Center Atmospheric Research (NCAR) - USA; University of Colorado System; University of Colorado Boulder; National Aeronautics & Space Administration (NASA); NASA Ames Research Center; National Aeronautics & Space Administration (NASA); NASA Langley Research Center; National Institute for Aerospace; University of California System; University of California Berkeley; University of California System; University of California Berkeley; ...
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Wolfe, Glenn M.,Hanisco, Thomas F.,Arkinson, Heather L.,et al. Photochemical evolution of the 2013 California Rim Fire: synergistic impacts of reactive hydrocarbons and enhanced oxidants[J],2022,22(6):23.
APA Wolfe, Glenn M..,Hanisco, Thomas F..,Arkinson, Heather L..,Blake, Donald R..,Wisthaler, Armin.,...&Cohen, Ronald C..(2022).Photochemical evolution of the 2013 California Rim Fire: synergistic impacts of reactive hydrocarbons and enhanced oxidants.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(6),23.
MLA Wolfe, Glenn M.,et al."Photochemical evolution of the 2013 California Rim Fire: synergistic impacts of reactive hydrocarbons and enhanced oxidants".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.6(2022):23.
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