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Observational Insights into Aerosol Formation from Isoprene

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Department of Environmental Science, Policy and Management, Department of Chemistry, University of California, Berkeley, California 94720, United States
Aerosol Dynamics Inc., Berkeley, California 94710, United States
§ Department of Environmental Sciences and Engineering, Gillings School of Global Public Health, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, United States
⊥ ○ Cooperative Institute for Research in the Environmental Sciences, Department of Biochemistry and Chemistry, University of Colorado, Boulder, Colorado 80309, United States
# NOAA Earth System Research Laboratory, Boulder, Colorado 80305, United States
Department of Atmospheric Sciences, Texas A&M University, College Station, Texas 77843, United States
California Institute of Technology, Pasadena, California 91125, United States
Department of Chemistry, University of Washington, Seattle, Washington 98195, United States
Scripps Institution of Oceanography, University of California, San Diego, La Jolla, California 92037, United States
Department of Chemistry, University of Aarhus, Aarhus, DK-8000, Denmark
Department of Atmospheric and Oceanic Sciences, Princeton University, Princeton, New Jersey 08544, United States
Geophysical Fluid Dynamics Laboratory, NOAA, Princeton, New Jersey 08540, United States
Air Resources Laboratory, NOAA, College Park, Maryland 20740, United States
Department of Meteorology, Pennsylvania State University, University Park, Pennsylvania 16802, United States
Departments of Environmental Science and Engineering and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, United States
$ Department of Civil and Environmental Engineering, University of California, Berkeley, California 94720, United States
% Now at Atmospheric Earth and Energy Division, Lawrence Livermore National Laboratory, Livermore, California 94550, United States
Now at Department of Atmospheric Environmental Sciences, Pusan National University, Busan, South Korea
Now at Institute of Arctic and Alpine Research, University of Colorado, Boulder, Colorado 80309, United States
Now at National Exposure Research Laboratory, Environmental Protection Agency, Research Triangle Park, North Carolina 27711, United States
° Now at Joint Center for Earth Systems Technology, University of Maryland and NASA Goddard Space Flight Center, Greenbelt, Maryland 20771, United States
Now at Department of Chemistry, Colorado State University, Fort Collins, Colorado 80523, United States
Now at ToFWerk AG, Thun, CH-3600, Switzerland
Now at Environmental Alion Science and Technology, EPA Office of Research and Development, EPA Research and Development, Research Triangle Park, North Carolina 27703, United States
+ Now at Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States
*E-mail: [email protected], Tel. +1-510-643-6449, Fax. +1-510-643-5098.
Cite this: Environ. Sci. Technol. 2013, 47, 20, 11403–11413
Publication Date (Web):September 4, 2013
Copyright © 2013 American Chemical Society

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    Abstract Image

    Atmospheric photooxidation of isoprene is an important source of secondary organic aerosol (SOA) and there is increasing evidence that anthropogenic oxidant emissions can enhance this SOA formation. In this work, we use ambient observations of organosulfates formed from isoprene epoxydiols (IEPOX) and methacrylic acid epoxide (MAE) and a broad suite of chemical measurements to investigate the relative importance of nitrogen oxide (NO/NO2) and hydroperoxyl (HO2) SOA formation pathways from isoprene at a forested site in California. In contrast to IEPOX, the calculated production rate of MAE was observed to be independent of temperature. This is the result of the very fast thermolysis of MPAN at high temperatures that affects the distribution of the MPAN reservoir (MPAN / MPA radical) reducing the fraction that can react with OH to form MAE and subsequently SOA (FMAE formation). The strong temperature dependence of FMAE formation helps to explain our observations of similar concentrations of IEPOX-derived organosulfates (IEPOX-OS; ∼1 ng m–3) and MAE-derived organosulfates (MAE-OS; ∼1 ng m–3) under cooler conditions (lower isoprene concentrations) and much higher IEPOX-OS (∼20 ng m–3) relative to MAE-OS (<0.0005 ng m–3) at higher temperatures (higher isoprene concentrations). A kinetic model of IEPOX and MAE loss showed that MAE forms 10−100 times more ring-opening products than IEPOX and that both are strongly dependent on aerosol water content when aerosol pH is constant. However, the higher fraction of MAE ring opening products does not compensate for the lower MAE production under warmer conditions (higher isoprene concentrations) resulting in lower formation of MAE-derived products relative to IEPOX at the surface. In regions of high NOx, high isoprene emissions and strong vertical mixing the slower MPAN thermolysis rate aloft could increase the fraction of MPAN that forms MAE resulting in a vertically varying isoprene SOA source.

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