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© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 18 Sep 2018

Research article | 18 Sep 2018

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This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Arctic marine secondary organic aerosol contributes significantly to summertime particle size distributions in the Canadian Arctic Archipelago

Betty Croft1, Randall V. Martin1,2, W. Richard Leaitch3, Julia Burkart4,a, Rachel Y.-W. Chang1, Douglas B. Collins4,b, Patrick L. Hayes5, Anna L. Hodshire6, Lin Huang3, John K. Kodros6, Alexander Moravek4, Emma L. Mungall4, Jennifer G. Murphy4, Sangeeta Sharma3, Samantha Tremblay5, Gregory R. Wentworth4,c, Megan D. Willis4, Jonathan P. D. Abbatt4, and Jeffrey R. Pierce6 Betty Croft et al.
  • 1Dalhousie University, Department of Physics and Atmospheric Science, Halifax, NS, B3H 4R2, Canada
  • 2Harvard-Smithsonian Center for Astrophysics, Cambridge, MA, 02138, USA
  • 3Environment and Climate Change Canada, Climate Research Division, Toronto, ON, M3H 5T4, Canada
  • 4University of Toronto, Department of Chemistry, Toronto, ON, M5S 3H6, Canada
  • 5Université de Montréal, Department of Chemistry, Montréal, QC, H3C 3J7, Canada
  • 6Colorado State University, Department of Atmospheric Science, Fort Collins, CO, 80423, USA
  • anow at: University of Vienna, Faculty of Physics, Aerosol Physics and Environmental Physics, Vienna, 1090, Austria
  • bnow at: Bucknell University, Department of Chemistry, Lewisburg, PA, 17837, USA
  • cnow at: Alberta Environment and Parks, Environmental Monitoring and Science Division, Edmonton, AB, T5J 5C6, Canada

Abstract. Summertime Arctic aerosol size distributions are strongly controlled by natural regional emissions. Within this context, we use a chemical transport model with size-resolved aerosol microphysics (GEOS-Chem-TOMAS) to interpret measurements of aerosol size distributions from the Canadian Arctic Archipelago during the summer of 2016, as part of the NETwork on Climate and Aerosols: addressing key uncertainties in Remote Canadian Environments (NETCARE). Our simulations suggest that condensation of secondary organic aerosol (SOA) from precursor vapors emitted in the Arctic and near Arctic marine (open ocean and coastal) regions plays a key role in particle growth events that shape the aerosol size distributions observed at Alert (82.5°N, 62.3°W), Eureka (80.1°N, 86.4°W), and along a NETCARE ship track within the Archipelago. We refer to this SOA as Arctic marine SOA (Arctic MSOA) to reflect the Arctic marine-based and likely biogenic sources for the precursors of the condensing organic vapors.

Arctic MSOA from a simulated flux (500μgm−2d−1, north of 50°N) of precursor vapors (assumed yield of unity) reduces the summertime particle size distribution model-observation mean fractional error by 2- to 4-fold, relative to a simulation without this Arctic MSOA. Particle growth due to the condensable organic vapor flux contributes strongly (30–50%) to the simulated summertime-mean number of particles with diameters larger than 20nm in the study region, and couples with ternary particle nucleation (sulfuric acid, ammonia, and water vapor) and biogenic sulfate condensation to account for more than 90% of this simulated particle number, a strong biogenic influence. The simulated fit to summertime size-distribution observations is further improved at Eureka and for the ship track by scaling up the nucleation rate by a factor of 100 to account for other particle precursors such as gas-phase iodine and/or amines and/or fragmenting primary particles that could be missing from our simulations. Additionally, the fits to observed size distributions and total aerosol number concentrations for particles larger than 4nm improve with the assumption that the Arctic MSOA contains semi-volatile species; reducing model-observation mean fractional error by 2- to 3-fold for the Alert and ship track size distributions. Arctic MSOA accounts for more than half of the simulated total particulate organic matter mass concentrations in the summertime Canadian Arctic Archipelago, and this Arctic MSOA has strong simulated summertime pan-Arctic-mean top-of-the-atmosphere aerosol direct (−0.04Wm−2) and cloud-albedo indirect (−0.4Wm−2) radiative effects. Future work should focus on further understanding summertime Arctic sources of Arctic MSOA.

Betty Croft et al.
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Status: final response (author comments only)
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Betty Croft et al.
Betty Croft et al.
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Short summary
Summertime Arctic atmospheric aerosols are strongly controlled by processes related to natural regional sources. We use a chemical transport model with size-resolved aerosol microphysics to interpret measurements made during summertime 2016 in the Canadian Arctic Archipelago. Our results explore the processes that control summertime aerosol size distributions and support a climate-relevant role for Arctic marine secondary organic aerosol formed from precursor vapors with Arctic marine sources.
Summertime Arctic atmospheric aerosols are strongly controlled by processes related to natural...