Abstract
Abstract. Urban areas are large sources of organic aerosols and their precursors. Nevertheless, the contributions of primary (POA) and secondary organic aerosol (SOA) to the observed particulate matter levels have been difficult to quantify. In this study the three-dimensional chemical transport model PMCAMx-2008 is used to investigate the temporal and geographic variability of organic aerosol in the Mexico City Metropolitan Area (MCMA) during the MILAGRO campaign that took place in the spring of 2006. The organic module of PMCAMx-2008 includes the recently developed volatility basis-set framework in which both primary and secondary organic components are assumed to be semi-volatile and photochemically reactive and are distributed in logarithmically spaced volatility bins. The MCMA emission inventory is modified and the POA emissions are distributed by volatility based on dilution experiments. The model predictions are compared with observations from four different types of sites, an urban (T0), a suburban (T1), a rural (T2), and an elevated site in Pico de Tres Padres (PTP). The performance of the model in reproducing organic mass concentrations in these sites is encouraging. The average predicted PM1 organic aerosol (OA) concentration in T0, T1, and T2 is 18 μg m−3, 11.7 μg m−3, and 10.5 μg m−3 respectively, while the corresponding measured values are 17.2 μg m−3, 11 μg m−3, and 9 μg m−3. The average predicted locally-emitted primary OA concentrations, 4.4 μg m−3 at T0, 1.2 μg m−3 at T1 and 1.7 μg m−3 at PTP, are in reasonably good agreement with the corresponding PMF analysis estimates based on the Aerosol Mass Spectrometer (AMS) observations of 4.5, 1.3, and 2.9 μg m−3 respectively. The model reproduces reasonably well the average oxygenated OA (OOA) levels in T0 (7.5 μg m−3 predicted versus 7.5 μg m−3 measured), in T1 (6.3 μg m−3 predicted versus 4.6 μg m−3 measured) and in PTP (6.6 μg m−3 predicted versus 5.9 μg m−3 measured). The rest of the OA mass (6.1 μg m−3 and 4.2 μg m−3 in T0 and T1 respectively) is assumed to originate from biomass burning activities and is introduced to the model as part of the boundary conditions. Inside Mexico City (at T0), the locally-produced OA is predicted to be on average 60 % locally-emitted primary (POA), 6 % semi-volatile (S-SOA) and intermediate volatile (I-SOA) organic aerosol, and 34 % traditional SOA from the oxidation of VOCs (V-SOA). The average contributions of the OA components to the locally-produced OA for the entire modelling domain are predicted to be 32 % POA, 10 % S-SOA and I-SOA, and 58 % V-SOA. The long range transport from biomass burning activities and other sources in Mexico is predicted to contribute on average almost as much as the local sources during the MILAGRO period.
Highlights
The Mexico City Metropolitan Area (MCMA) is the largest megacity in North America and is one of the five largest cities in the world with over 20 million people living in an area of Published by Copernicus Publications on behalf of the European Geosciences Union.A
At T1 and T2, OOA corresponds to 60 % and 85 % of locally-produced organic aerosol (OA) respectively
V-secondary organic aerosol (SOA) is predicted to be the dominant component of OOA as the emission rate of its precursors is more than ten times higher than the I-VOC and S-VOC emission rate (Table 1)
Summary
The Mexico City Metropolitan Area (MCMA) is the largest megacity in North America and is one of the five largest cities in the world with over 20 million people living in an area of Published by Copernicus Publications on behalf of the European Geosciences Union. Aiken et al (2010) estimated that during the low regional fire periods, 38 % of OC in the Mexico City center was from non-fossil sources, suggesting the importance of urban and regional non-fossil carbon sources other than the fires, such as food cooking and regional biogenic SOA They showed that, by properly accounting for the non-BB sources of K, the fires from the region near the MCMA are estimated to contribute 15–23 % of the OA. Hodzic et al (2010) applied the CHIMERE model to estimate the potential contribution to SOA formation of recently identified semi-volatile and intermediate volatility organic precursors (Robinson et al, 2007) in and around Mexico City Their results showed a substantial enhancement in predicted SOA concentrations (2–4 times) both within and downwind of the city leading to much reduced discrepancies with the total OA measurements.
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