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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
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Volume 15, issue 6
Atmos. Chem. Phys., 15, 3063-3075, 2015
https://doi.org/10.5194/acp-15-3063-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
Atmos. Chem. Phys., 15, 3063-3075, 2015
https://doi.org/10.5194/acp-15-3063-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 18 Mar 2015

Research article | 18 Mar 2015

Effect of oxidant concentration, exposure time, and seed particles on secondary organic aerosol chemical composition and yield

A. T. Lambe2,1, P. S. Chhabra2,*, T. B. Onasch2,1, W. H. Brune3, J. F. Hunter4, J. H. Kroll4, M. J. Cummings1, J. F. Brogan1, Y. Parmar1, D. R. Worsnop2, C. E. Kolb2, and P. Davidovits1 A. T. Lambe et al.
  • 1Chemistry Department, Boston College, Chestnut Hill, MA, USA
  • 2Aerodyne Research Inc., Billerica, MA, USA
  • 3Department of Meteorology and Atmospheric Sciences, Pennsylvania State University, State College, PA, USA
  • 4Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA
  • *now at: Department of Chemical Engineering, University of Texas, Austin, Texas, USA

Abstract. We performed a systematic intercomparison study of the chemistry and yields of secondary organic aerosol (SOA) generated from OH oxidation of a common set of gas-phase precursors in a Potential Aerosol Mass (PAM) continuous flow reactor and several environmental chambers. In the flow reactor, SOA precursors were oxidized using OH concentrations ranging from 2.0 × 108 to 2.2 × 1010 molec cm−3 over exposure times of 100 s. In the environmental chambers, precursors were oxidized using OH concentrations ranging from 2 × 106 to 2 × 107 molec cm−3 over exposure times of several hours. The OH concentration in the chamber experiments is close to that found in the atmosphere, but the integrated OH exposure in the flow reactor can simulate atmospheric exposure times of multiple days compared to chamber exposure times of only a day or so. In most cases, for a specific SOA type the most-oxidized chamber SOA and the least-oxidized flow reactor SOA have similar mass spectra, oxygen-to-carbon and hydrogen-to-carbon ratios, and carbon oxidation states at integrated OH exposures between approximately 1 × 1011 and 2 × 1011 molec cm−3 s, or about 1–2 days of equivalent atmospheric oxidation. This observation suggests that in the range of available OH exposure overlap for the flow reactor and chambers, SOA elemental composition as measured by an aerosol mass spectrometer is similar whether the precursor is exposed to low OH concentrations over long exposure times or high OH concentrations over short exposure times. This similarity in turn suggests that both in the flow reactor and in chambers, SOA chemical composition at low OH exposure is governed primarily by gas-phase OH oxidation of the precursors rather than heterogeneous oxidation of the condensed particles. In general, SOA yields measured in the flow reactor are lower than measured in chambers for the range of equivalent OH exposures that can be measured in both the flow reactor and chambers. The influence of sulfate seed particles on isoprene SOA yield measurements was examined in the flow reactor. The studies show that seed particles increase the yield of SOA produced in flow reactors by a factor of 3 to 5 and may also account in part for higher SOA yields obtained in the chambers, where seed particles are routinely used.

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We compared the chemistry and yields of SOA generated from OH oxidation of gas-phase precursors in a flow reactor (high OH, short residence time) and environmental chambers (low OH, long residence time). We find that chemical composition of SOA produced in the flow reactor and in chambers is similar. SOA yields measured in the flow reactor are lower than in chambers. Seed particles increase the yield of SOA produced in the flow reactor and may account in part for higher SOA yields in chambers.
We compared the chemistry and yields of SOA generated from OH oxidation of gas-phase precursors...
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