Aerosols from anthropogenic and biogenic sources and their interactions – modeling aerosol formation, optical properties, and impacts over the central Amazon basin

摘要

The Green Ocean Amazon experiment – GoAmazon 2014–2015 – explored the interactions between natural biogenic forest emissions from central Amazonia and urban air pollution from Manaus. Previous GoAmazon 2014–2015 studies showed that nitrogen oxide (NO x ? = ?NO? + ?NO 2 ) and sulfur oxide (SO x ) emissions from Manaus strongly interact with biogenic volatile organic compounds (BVOCs), affecting secondary organic aerosol (SOA) formation. In previous studies, ground-based and aircraft measurements provided evidence of SOA formation and strong changes in aerosol composition and properties. Aerosol optical properties also evolve, and their impacts on the Amazonian ecosystem can be significant. As particles age, some processes, such as SOA production, black carbon (BC) deposition, particle growth and the BC lensing effect change the aerosol optical properties, affecting the solar radiation flux at the surface. This study analyzes data and models SOA formation using the Weather Research and Forecasting with Chemistry (WRF-Chem) model to assess the spatial variability in aerosol optical properties as the Manaus plumes interact with the natural atmosphere. The following aerosol optical properties are investigated: single scattering albedo (SSA), asymmetry parameter ( g aer ), absorption ?ngstr?m exponent (AAE) and scattering ?ngstr?m exponent (SAE). These simulations were validated using ground-based measurements at three experimental sites, namely the Amazon Tall Tower Observatory – ATTO (T0a), downtown Manaus (T1), Tiwa Hotel (T2) and Manacapuru (T3), as well as the U.S. Department of Energy (DOE) Gulfstream 1 (G-1) aircraft flights. WRF-Chem simulations were performed over 7?d during March 2014. Results show a mean biogenic SOA (BSOA) mass enrichment of 512?% at the T1 site, 450?% in regions downwind of Manaus, such as the T3 site, and 850?% in areas north of the T3 site in simulations with anthropogenic emissions. The SOA formation is rather fast, with about 80?% of the SOA mass produced in 3–4?h. Comparing the plume from simulations with and without anthropogenic emissions, SSA shows a downwind reduction of approximately 10?%, 11?% and 6?% at the T1, T2 and T3 sites, respectively. Other regions, such as those further downwind of the T3 site, are also affected. The g aer values increased from 0.62 to 0.74 at the T1 site and from 0.67 to 0.72 at the T3 site when anthropogenic emissions are active. During the Manaus plume-aging process, a plume tracking analysis shows an increase in SSA from 0.91 close to Manaus to 0.98 160?km downwind of Manaus as a result of SOA production and BC deposition.