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Discussion papers
https://doi.org/10.5194/acp-2019-331
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2019-331
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 06 May 2019

Research article | 06 May 2019

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

An evaluation of global organic aerosol schemes using airborne observations

Sidhant J. Pai1, Colette L. Heald1,2, Jeffrey R. Pierce3, Salvatore C. Farina3, Eloise A. Marais4, Jose L. Jimenez5, Pedro Campuzano-Jost5, Benjamin A. Nault5, Ann M. Middlebrook6, Hugh Coe7, John E. Shilling8, Roya Bahreini9, Justin H. Dingle9, and Kennedy Vu9 Sidhant J. Pai et al.
  • 1Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, Cambridge, MA, 02139, USA
  • 2Department of Earth, Atmospheric and Planetary Sciences, Massachusetts Institute of Technology, Cambridge, MA, 02139, USA
  • 3Colorado State University, Department of Atmospheric Science, Fort Collins, CO, 80523, USA
  • 4Department of Physics and Astronomy, University of Leicester, Leicester, LE1 7RH, UK
  • 5Department ofChemistry, and Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, CO, 80309, USA
  • 6NOAA Earth System Research Laboratory (ESRL) Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
  • 7Centre forAtmospheric Science, School of Earth and Environmental Science, University of Manchester, Manchester, M13 9PL, UK
  • 8Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland, Washington, USA
  • 9Department of Environmental Sciences, University of California, Riverside, CA 92521, USA

Abstract. Chemical transport models have historically struggled to accurately simulate the magnitude and variability of observed organic aerosol (OA), with previous studies demonstrating that models significantly underestimate observed concentrations in the troposphere. In this study, we explore two different model OA schemes within the standard GEOS-Chem chemical transport model and evaluate the simulations against a suite of 15 globally-distributed airborne campaigns from 2008–2017. These include the ATom, KORUS-AQ, GoAmazon, FRAPPE, SEAC4RS, SENEX, DC3, CalNex, OP3, EUCAARI, ARCTAS and ARCPAC campaigns and provide broad coverage over a diverse set of atmospheric-composition regimes – anthropogenic, biogenic, pyrogenic and remote. The schemes include significant differences in their treatment of the primary and secondary components of OA – a simple scheme that models primary OA (POA) as non-volatile and takes a fixed-yield approach to secondary OA (SOA) formation, and a complex scheme that simulates POA as semi-volatile and uses a more sophisticated volatility basis set approach for non-isoprene SOA, with an explicit aqueous uptake mechanism to model isoprene SOA. Despite these substantial differences, both the simple and complex schemes perform comparably across the aggregate dataset in their ability to capture the observed variability (with an R2 of 0.41 and 0.44 respectively). The simple scheme displays greater skill in minimizing the overall model-bias (with a NMB of 0.04, compared to 0.29 for the complex scheme). Across both schemes, the model skill in reproducing observed OA is superior to previous model evaluations and approaches the fidelity of the sulfate simulation within GEOS-Chem. However, there are significant differences in model performance across different chemical source regimes, classified here into 7 categories. Higher-resolution nested regional simulations indicate that model resolution is an important factor in capturing variability in highly-localized campaigns, while also demonstrating the importance of well-constrained emissions inventories and local meteorology, particularly over Asia. A comparison of the POA loadings from the complex scheme with SOA loadings from the simple scheme (and vice versa) also suggests that a semi-volatile treatment of POA is superior to a non-volatile treatment. While this study identifies factors within the SOA schemes that likely contribute to OA model bias (such as a strong dependency of the bias in the complex scheme on relative humidity and sulfate concentrations), comparisons with the skill of the sulfate aerosol scheme in GEOS-Chem indicate the importance of other drivers of bias such as emissions, transport, and deposition that are exogenous to the OA chemical scheme.

Sidhant J. Pai et al.
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Status: final response (author comments only)
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Short summary
Aerosols in the atmosphere have significant health and climate impacts. Organic aerosol (OA) accounts for a large fraction of the total aerosol burden, but models have historically struggled to accurately simulate it. This study compares two very different OA model schemes and evaluates them against a suite of globally-distributed airborne measurements with the goal of providing insight into the strengths and weaknesses of each approach across different environments.
Aerosols in the atmosphere have significant health and climate impacts. Organic aerosol (OA)...
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