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Atmos Chem Phys
| Title: | Organic nitrate chemistry and its implications for nitrogen budgets in an isoprene- and monoterpene-rich atmosphere: constraints from aircraft (SEAC(4)RS) and ground-based (SOAS) observations in the Southeast US |
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| Author(s): | Fisher JA; Jacob DJ; Travis KR; Kim PS; Marais EA; Miller CC; Yu K; Zhu L; Yantosca RM; Sulprizio MP; Mao J; Wennberg PO; Crounse JD; Teng AP; Nguyen TB; St Clair JM; Cohen RC; Romer P; Nault BA; Wooldridge PJ; Jimenez JL; Campuzano-Jost P; Day DA; Hu W; Shepson PB; Xiong F; Blake DR; Goldstein AH; Misztal PK; Hanisco TF; Wolfe GM; Ryerson TB; Wisthaler A; Mikoviny T; |
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| Address: | "Centre for Atmospheric Chemistry, School of Chemistry, University of Wollongong, Wollongong, NSW, Australia. School of Earth and Environmental Sciences, University of Wollongong, Wollongong, NSW, Australia. Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA. Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA, USA. Program in Atmospheric and Oceanic Sciences, Princeton University, Princeton, NJ, USA. Geophysical Fluid Dynamics Laboratory/National Oceanic and Atmospheric Administration, Princeton, NJ, USA. Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA. Division of Engineering and Applied Science, California Institute of Technology, Pasadena, CA, USA. Now at Department of Environmental Toxicology, University of California at Davis, Davis, CA, USA. Now at Atmospheric Chemistry and Dynamics Laboratory, NASA Goddard Space Flight Center, Greenbelt, MD, USA and Joint Center for Earth Systems Technology, University of Maryland Baltimore County, Baltimore, MD, USA. Department of Chemistry, University of California at Berkeley, Berkeley, CA, USA. Department of Earth and Planetary Science, University of California at Berkeley, Berkeley, CA, USA. Now at Department of Chemistry and Biochemistry and Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA. Department of Chemistry and Biochemistry, University of Colorado, Boulder, CO, USA. Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA. Department of Chemistry, Purdue University, West Lafayette, IN, USA. Department of Earth, Atmospheric and Planetary Sciences, Purdue University, West Lafayette, IN, USA. Department of Chemistry, University of California Irvine, Irvine, CA, USA. Department of Environmental Science, Policy, and Management, University of California at Berkeley, Berkeley, CA, USA. Department of Civil and Environmental Engineering, University of California at Berkeley, Berkeley, CA, USA. Atmospheric Chemistry and Dynamics Laboratory, NASA Goddard Space Flight Center, Greenbelt, MD, USA. Joint Center for Earth Systems Technology, University of Maryland Baltimore County, Baltimore, MD, USA. Chemical Sciences Division, Earth System Research Lab, National Oceanic and Atmospheric Administration, Boulder, CO, USA. Department of Chemistry, University of Oslo, Oslo, Norway. Institute for Ion Physics and Applied Physics, University of Innsbruck, Innsbruck, Austria" |
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| Journal Title: | Atmos Chem Phys |
| Year: | 2016 |
| Volume: | 20160517 |
| Issue: | 9 |
| Page Number: | 5969 - 5991 |
| DOI: | 10.5194/acp-16-5969-2016 |
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| ISSN/ISBN: | 1680-7316 (Print) 1680-7324 (Electronic) 1680-7316 (Linking) |
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| Abstract: | "Formation of organic nitrates (RONO(2)) during oxidation of biogenic volatile organic compounds (BVOCs: isoprene, monoterpenes) is a significant loss pathway for atmospheric nitrogen oxide radicals (NO(x)), but the chemistry of RONO(2) formation and degradation remains uncertain. Here we implement a new BVOC oxidation mechanism (including updated isoprene chemistry, new monoterpene chemistry, and particle uptake of RONO(2)) in the GEOS-Chem global chemical transport model with approximately 25 x 25 km(2) resolution over North America. We evaluate the model using aircraft (SEAC(4)RS) and ground-based (SOAS) observations of NO(x), BVOCs, and RONO(2) from the Southeast US in summer 2013. The updated simulation successfully reproduces the concentrations of individual gas- and particle-phase RONO(2) species measured during the campaigns. Gas-phase isoprene nitrates account for 25-50% of observed RONO(2) in surface air, and we find that another 10% is contributed by gas-phase monoterpene nitrates. Observations in the free troposphere show an important contribution from long-lived nitrates derived from anthropogenic VOCs. During both campaigns, at least 10% of observed boundary layer RONO(2) were in the particle phase. We find that aerosol uptake followed by hydrolysis to HNO(3) accounts for 60% of simulated gas-phase RONO(2) loss in the boundary layer. Other losses are 20% by photolysis to recycle NO(x) and 15% by dry deposition. RONO(2) production accounts for 20% of the net regional NO(x) sink in the Southeast US in summer, limited by the spatial segregation between BVOC and NO(x) emissions. This segregation implies that RONO(2) production will remain a minor sink for NO(x) in the Southeast US in the future even as NO(x) emissions continue to decline" |
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| Notes: | "PubMed-not-MEDLINEFisher, J A Jacob, D J Travis, K R Kim, P S Marais, E A Miller, C Chan Yu, K Zhu, L Yantosca, R M Sulprizio, M P Mao, J Wennberg, P O Crounse, J D Teng, A P Nguyen, T B St Clair, J M Cohen, R C Romer, P Nault, B A Wooldridge, P J Jimenez, J L Campuzano-Jost, P Day, D A Hu, W Shepson, P B Xiong, F Blake, D R Goldstein, A H Misztal, P K Hanisco, T F Wolfe, G M Ryerson, T B Wisthaler, A Mikoviny, T eng Germany 2016/01/01 Atmos Chem Phys. 2016; 16(9):5969-5991. doi: 10.5194/acp-16-5969-2016. Epub 2016 May 17" |
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