References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-10-5491-2010

Modeling organic aerosols in a megacity: potential contribution of semi-volatile and intermediate volatility primary organic compounds to secondary organic aerosol formation

Hodzic

¹ Jimenez

J. L.

² Madronich

¹ Canagaratna

M. R.

³ DeCarlo

P. F.

² ⁴ ⁷ Kleinman

⁵ Fast

⁶

National Center for Atmospheric Research, Boulder, CO, USA

Dept. of Chemistry and Biochemistry, and CIRES, Univ. of Colorado, Boulder, CO, USA

Aerodyne Research, Billerica, MA, USA

Dept. of Atmospheric and Oceanic Science, Univ. of Colorado, Boulder, CO, USA

Brookhaven National Laboratory, Upton, New York, USA

Pacific Northwest National Laboratory, Richland, WA, USA

now at: Laboratory of Atmospheric Chemistry, Paul Scherrer Institut, Villigen, Switzerland

21 06 2010

10 12 5491 5514

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

This article is available from http://www.atmos-chem-phys.net/10/5491/2010/acp-10-5491-2010.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/10/5491/2010/acp-10-5491-2010.pdf

It has been established that observed local and regional levels of secondary organic aerosols (SOA) in polluted areas cannot be explained by the oxidation and partitioning of anthropogenic and biogenic VOC precursors, at least using current mechanisms and parameterizations. In this study, the 3-D regional air quality model CHIMERE is applied to estimate the potential contribution to SOA formation of recently identified semi-volatile and intermediate volatility organic precursors (S/IVOC) in and around Mexico City for the MILAGRO field experiment during March 2006. The model has been updated to include explicitly the volatility distribution of primary organic aerosols (POA), their gas-particle partitioning and the gas-phase oxidation of the vapors. Two recently proposed parameterizations, those of Robinson et al. (2007) ("ROB") and Grieshop et al. (2009) ("GRI") are compared and evaluated against surface and aircraft measurements. The 3-D model results are assessed by comparing with the concentrations of OA components from Positive Matrix Factorization of Aerosol Mass Spectrometer (AMS) data, and for the first time also with oxygen-to-carbon ratios derived from high-resolution AMS measurements. The results show a substantial enhancement in predicted SOA concentrations (2–4 times) with respect to the previously published base case without S/IVOCs (Hodzic et al., 2009), both within and downwind of the city leading to much reduced discrepancies with the total OA measurements. Model improvements in OA predictions are associated with the better-captured SOA magnitude and diurnal variability. The predicted production from anthropogenic and biomass burning S/IVOC represents 40–60% of the total measured SOA at the surface during the day and is somewhat larger than that from commonly measured aromatic VOCs, especially at the T1 site at the edge of the city. The SOA production from the continued multi-generation S/IVOC oxidation products continues actively downwind. Similar to aircraft observations, the predicted OA/ΔCO ratio for the ROB case increases from 20–30 μg sm−3 ppm−1 up to 60–70 μg sm−3 ppm−1 between a fresh and 1-day aged air mass, while the GRI case produces a 30% higher OA growth than observed. The predicted average O/C ratio of total OA for the ROB case is 0.16 at T0, substantially below observed value of 0.5. A much better agreement for O/C ratios and temporal variability (R2=0.63) is achieved with the updated GRI treatment. Both treatments show a deficiency in regard to POA ageing with a tendency to over-evaporate POA upon dilution of the urban plume suggesting that atmospheric HOA may be less volatile than assumed in these parameterizations. This study highlights the important potential role of S/IVOC chemistry in the SOA budget in this region, and highlights the need for further improvements in available parameterizations. The agreement observed in this study is not sufficient evidence to conclude that S/IVOC are the major missing SOA source in megacity environments. The model is still very underconstrained, and other possible pathways such as formation from very volatile species like glyoxal may explain some of the mass and especially increase the O/C ratio.

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