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Lee BH, Mohr C, Lopez-Hilfiker FD, et al. Highly functionalized organic nitrates in the southeast United States: Contribution to secondary organic aerosol and reactive nitrogen budgets. Proc Natl Acad Sci U S A. 2016;113(6):1516-21doi: 10.1073/pnas.1508108113.
Lee, B. H., Mohr, C., Lopez-Hilfiker, F. D., Lutz, A., Hallquist, M., Lee, L., Romer, P., Cohen, R. C., Iyer, S., Kurtén, T., Hu, W., Day, D. A., Campuzano-Jost, P., Jimenez, J. L., Xu, L., Ng, N. L., Guo, H., Weber, R. J., Wild, R. J., Brown, S. S., Koss, A., de Gouw, J., Olson, K., Goldstein, A. H., Seco, R., Kim, S., McAvey, K., Shepson, P. B., Starn, T., Baumann, K., Edgerton, E. S., Liu, J., Shilling, J. E., Miller, D. O., Brune, W., Schobesberger, S., D'Ambro, E. L., & Thornton, J. A. (2016). Highly functionalized organic nitrates in the southeast United States: Contribution to secondary organic aerosol and reactive nitrogen budgets. Proceedings of the National Academy of Sciences of the United States of America, 113(6), 1516-21. https://doi.org/10.1073/pnas.1508108113
Lee, Ben H, et al. "Highly functionalized organic nitrates in the southeast United States: Contribution to secondary organic aerosol and reactive nitrogen budgets." Proceedings of the National Academy of Sciences of the United States of America vol. 113,6 (2016): 1516-21. doi: https://doi.org/10.1073/pnas.1508108113
Lee BH, Mohr C, Lopez-Hilfiker FD, Lutz A, Hallquist M, Lee L, Romer P, Cohen RC, Iyer S, Kurtén T, Hu W, Day DA, Campuzano-Jost P, Jimenez JL, Xu L, Ng NL, Guo H, Weber RJ, Wild RJ, Brown SS, Koss A, de Gouw J, Olson K, Goldstein AH, Seco R, Kim S, McAvey K, Shepson PB, Starn T, Baumann K, Edgerton ES, Liu J, Shilling JE, Miller DO, Brune W, Schobesberger S, D'Ambro EL, Thornton JA. Highly functionalized organic nitrates in the southeast United States: Contribution to secondary organic aerosol and reactive nitrogen budgets. Proc Natl Acad Sci U S A. 2016 Feb 09;113(6):1516-21. doi: 10.1073/pnas.1508108113. Epub 2016 Jan 25. PMID: 26811465; PMCID: PMC4760802.
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Proc Natl Acad Sci U S A. 2016 Feb 09;113(6):1516-21. doi: 10.1073/pnas.1508108113. Epub 2016 Jan 25.

Highly functionalized organic nitrates in the southeast United States: Contribution to secondary organic aerosol and reactive nitrogen budgets.

Proceedings of the National Academy of Sciences of the United States of America

Ben H Lee, Claudia Mohr, Felipe D Lopez-Hilfiker, Anna Lutz, Mattias Hallquist, Lance Lee, Paul Romer, Ronald C Cohen, Siddharth Iyer, Theo Kurtén, Weiwei Hu, Douglas A Day, Pedro Campuzano-Jost, Jose L Jimenez, Lu Xu, Nga Lee Ng, Hongyu Guo, Rodney J Weber, Robert J Wild, Steven S Brown, Abigail Koss, Joost de Gouw, Kevin Olson, Allen H Goldstein, Roger Seco, Saewung Kim, Kevin McAvey, Paul B Shepson, Tim Starn, Karsten Baumann, Eric S Edgerton, Jiumeng Liu, John E Shilling, David O Miller, William Brune, Siegfried Schobesberger, Emma L D'Ambro, Joel A Thornton

Affiliations

  1. Department of Atmospheric Sciences, University of Washington, Seattle, WA 98195;
  2. Department of Chemistry and Molecular Biology, Atmospheric Science, University of Gothenburg, SE-41296 Gothenburg, Sweden;
  3. Department of Chemistry, University of California, Berkeley, CA 94720;
  4. Department of Chemistry, Laboratory of Physical Chemistry, University of Helsinki, Helsinki FIN-00014, Finland;
  5. Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder, CO 80309; Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309;
  6. School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA 30332;
  7. School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA 30332; School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA 30332;
  8. School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA 30332;
  9. Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309; Chemical Sciences Division, National Oceanic and Atmospheric Administration, Boulder, CO 80305;
  10. Chemical Sciences Division, National Oceanic and Atmospheric Administration, Boulder, CO 80305;
  11. Department of Environmental Science, Policy and Management, University of California, Berkeley, CA 94720;
  12. Department of Earth System Science, School of Physical Sciences, University of California, Irvine, CA 92697;
  13. Departments of Chemistry and Earth, Atmospheric and Planetary Sciences and Purdue Climate Change Research Center, Purdue University, West Lafayette, IN 47907;
  14. Department of Chemistry, West Chester University, West Chester, PA 19383;
  15. Atmospheric Research and Analysis, Inc., Cary, NC 27513;
  16. Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland, WA 99352;
  17. Department of Meteorology, Pennsylvania State University, University Park, PA 16802;
  18. Department of Chemistry, University of Washington, Seattle, WA 98195.
  19. Department of Atmospheric Sciences, University of Washington, Seattle, WA 98195; [email protected].

PMID: 26811465 PMCID: PMC4760802 DOI: 10.1073/pnas.1508108113

Abstract

Speciated particle-phase organic nitrates (pONs) were quantified using online chemical ionization MS during June and July of 2013 in rural Alabama as part of the Southern Oxidant and Aerosol Study. A large fraction of pONs is highly functionalized, possessing between six and eight oxygen atoms within each carbon number group, and is not the common first generation alkyl nitrates previously reported. Using calibrations for isoprene hydroxynitrates and the measured molecular compositions, we estimate that pONs account for 3% and 8% of total submicrometer organic aerosol mass, on average, during the day and night, respectively. Each of the isoprene- and monoterpenes-derived groups exhibited a strong diel trend consistent with the emission patterns of likely biogenic hydrocarbon precursors. An observationally constrained diel box model can replicate the observed pON assuming that pONs (i) are produced in the gas phase and rapidly establish gas-particle equilibrium and (ii) have a short particle-phase lifetime (∼2-4 h). Such dynamic behavior has significant implications for the production and phase partitioning of pONs, organic aerosol mass, and reactive nitrogen speciation in a forested environment.

Keywords: biogenic volatile organic compound oxidation; high-resolution time-of-flight chemical ionization mass spectrometer; lifetime calculation; online measurement; particulate organic nitrates

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