PNNL

Abstract

The Green Ocean Amazon (GoAmazon 2014/5) campaign, conducted from January 2014 – December 2015 in the vicinity of Manaus, Brazil, was designed to study the aerosol lifecycle and aerosol-cloud interactions in both pristine and anthropogenically-influenced conditions. As part of this campaign, the U.S. Department of Energy (DOE) G-1 research aircraft was deployed from February 17 – March 25, 2014 (wet season) and September 6 – October 5, 2014 (dry season) to investigate aerosol and cloud properties aloft. Here, we present results from the G-1 deployments focusing on measurements of the aerosol chemical composition and discussion of aerosol sources and secondary organic aerosol formation and aging. In the first portion of the manuscript, we provide an overview of the data and compare and contrast the data from the wet and dry season. Organic aerosol (OA) dominates the deployment-averaged chemical composition, comprising 78% of the total mass with sulfate comprising 12%, nitrate 5%, and ammonium 4%. This product distribution was unchanged between seasons, despite the fact that total aerosol loading was significantly higher in the dry season and that regional and local biomass burning was a significant source of OA mass in the dry, but not wet, season. However, the OA was more oxidized in the dry season, with the median of the mean carbon oxidation state increasing from -0.45 in the wet season to -0.02 in the dry season. In the second portion of the manuscript, we discuss the evolution of the Manaus plume on March 13, 2014, one of the golden days in the wet season. On this flight, we observe a clear increase in OA concentrations in the Manaus plume relative to the background. As the plume is transported downwind and ages, we observe dynamic changes in the OA. The mean carbon oxidation state of the OA increases from -0.6 to -0.45 during the 4-5 hours of photochemical aging. Hydrocarbon-like organic aerosol (HOA) mass is lost with ?HOA/?CO values decreasing from 17.6 µg/m3 ppmv-1 over Manaus to 10.6 µg/m3 ppmv-1 95 km downwind. Loss of HOA is balanced out by formation of oxygenated organic aerosol (OOA) with ?OOA/?CO increasing from 9.2 to 23.1 µg/m3 ppmv-1. Because HOA loss is balanced by OOA formation, we observe little change in the net ?org/?CO values; ?org/?CO averages 31 µg/m3 ppmv-1 and does not increase with aging. Our observation of constant ?org/?CO are in contrast to literature studies of the outflow of several North American cities, which report significant increases in ?org/?CO for the first day of plume aging. These observations suggest that SOA formation in the Manaus plume occurs, at least in part, by a different mechanism than observed in urban outflow plumes in most other literature studies. Constant ?org/?CO with plume aging has been observed in many biomass burning plumes, but we are unaware of reports of fresh urban emissions aging in this manner. These observations show that urban pollution emitted from Manaus in the wet season forms much less particulate downwind than urban pollution emitted from North American cities.