Abstract
Abstract. As a contribution to the Large-Scale Biosphere-Atmosphere Experiment in Amazonia – Cooperative LBA Airborne Regional Experiment (LBA-CLAIRE-2001) field campaign in the heart of the Amazon Basin, we analyzed the temporal and spatial dynamics of the urban plume of Manaus City during the wet-to-dry season transition period in July 2001. During the flights, we performed vertical stacks of crosswind transects in the urban outflow downwind of Manaus City, measuring a comprehensive set of trace constituents including O3, NO, NO2, CO, VOC, CO2, and H2O. Aerosol loads were characterized by concentrations of total aerosol number (CN) and cloud condensation nuclei (CCN), and by light scattering properties. Measurements over pristine rainforest areas during the campaign showed low levels of pollution from biomass burning or industrial emissions, representative of wet season background conditions. The urban plume of Manaus City was found to be joined by plumes from power plants south of the city, all showing evidence of very strong photochemical ozone formation. One episode is discussed in detail, where a threefold increase in ozone mixing ratios within the atmospheric boundary layer occurred within a 100 km travel distance downwind of Manaus. Observation-based estimates of the ozone production rates in the plume reached 15 ppb h−1. Within the plume core, aerosol concentrations were strongly enhanced, with ΔCN/ΔCO ratios about one order of magnitude higher than observed in Amazon biomass burning plumes. ΔCN/ΔCO ratios tended to decrease with increasing transport time, indicative of a significant reduction in particle number by coagulation, and without substantial new particle nucleation occurring within the time/space observed. While in the background atmosphere a large fraction of the total particle number served as CCN (about 60–80% at 0.6% supersaturation), the CCN/CN ratios within the plume indicated that only a small fraction (16±12%) of the plume particles were CCN. The fresh plume aerosols showed relatively weak light scattering efficiency. The CO-normalized CCN concentrations and light scattering coefficients increased with plume age in most cases, suggesting particle growth by condensation of soluble organic or inorganic species. We used a Single Column Chemistry and Transport Model (SCM) to infer the urban pollution emission fluxes of Manaus City, implying observed mixing ratios of CO, NOx and VOC. The model can reproduce the temporal/spatial distribution of ozone enhancements in the Manaus plume, both with and without accounting for the distinct (high NOx) contribution by the power plants; this way examining the sensitivity of ozone production to changes in the emission rates of NOx. The VOC reactivity in the Manaus region was dominated by a high burden of biogenic isoprene from the background rainforest atmosphere, and therefore NOx control is assumed to be the most effective ozone abatement strategy. Both observations and models show that the agglomeration of NOx emission sources, like power plants, in a well-arranged area can decrease the ozone production efficiency in the near field of the urban populated cores. But on the other hand remote areas downwind of the city then bear the brunt, being exposed to increased ozone production and N-deposition. The simulated maximum stomatal ozone uptake fluxes were 4 nmol m−2 s−1 close to Manaus, and decreased only to about 2 nmol m−2 s−1 within a travel distance >1500 km downwind from Manaus, clearly exceeding the critical threshold level for broadleaf trees. Likewise, the simulated N deposition close to Manaus was ~70 kg N ha−1 a−1 decreasing only to about 30 kg N ha−1 a−1 after three days of simulation.
Highlights
Tropical regions play a central role in the budgets of trace gases and aerosols of the Earth’s atmosphere, as well as in the absorption of solar energy and its transfer into the climate system
To characterize the background conditions in the Manaus region during the wet-to-dry season transition period, vertical profiles of observed mixing ratios for carbon monoxide (CO), Nitric oxide (NO), O3, CO2, H2O, CN, CCN0.6, and the potential temperature from Flight #18 are shown in Fig. 3; and for isoprene and α-pinene the mean vertical profiles from 8 background flights during the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA)-CLAIRE2001 are shown
volatile organic compounds (VOCs) compete with NO2 for the OH radicals, and the generated peroxy radicals convert NO into NO2, leading to O3 production
Summary
Tropical regions play a central role in the budgets of trace gases and aerosols of the Earth’s atmosphere, as well as in the absorption of solar energy and its transfer into the climate system. Amongst the most important anthropogenic pollutants are nitrogen oxides (NOx = sum of nitric oxide [NO] and nitrogen dioxide [NO2]), volatile organic compounds (VOCs), carbon monoxide (CO) and aerosols, all of which drive the formation of photochemical smog and control the photochemical production of tropospheric ozone (O3) and the hydroxyl radical (OH) These oxidants play a key role in determining the oxidizing power of the global atmosphere, and the capacity of the atmosphere to cleanse itself; while on the other hand their build-up by photochemical air pollution may threaten both human and ecosystem health on regional and continental scales. Because of the large biogenic background sources of VOC, which act as key precursors for SOA formation, a potentially important production of secondary organic aerosol (SOA) is anticipated for tropical urban plumes. The results are used to examine the impacts of urbanization on the net exchange and atmospheric chemistry of important gases and aerosols, and to provide scientific insights in the potential consequences and efficiencies of emission abatement strategies
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