Abstract. We present a range of airborne in-situ observations of biomass burning carbonaceous aerosol over tropical South America, including a case study of a large tropical forest wildfire and a series of regional survey flights across the Brazilian Amazon and Cerrado. The study forms part of the South American Biomass Burning Analysis (SAMBBA) Project, which was conducted during September and October 2012. We find limited evidence for net increases in aerosol mass through atmospheric aging combined with substantial changes in the chemical properties of organic aerosol (OA). Oxidation of the OA increases significantly and rapidly on the scale of 2.5–3 hours based on our case study analysis and is consistent with secondary organic aerosol production. The observations of limited net enhancement in OA coupled with such changes in chemical composition, imply that evaporation of OA is also occurring to balance these changes. We observe significant coatings on black carbon particles at source, but with limited changes with aging in both particle core size and coating thickness. We quantify variability in the ratio of OA to carbon monoxide across our study as a key parameter representing both initial fire conditions and an indicator of net aerosol production with atmospheric aging. We observe ratios of 0.075–0.13 μg sm−3 ppbv−1 in the west of our study region over the Amazon tropical forest in air masses less influenced by precipitation and a value of 0.095 μg sm−3 ppbv−1 over the Cerrado environment in the east. Such values are consistent with emission factors used by numerical models to represent biomass burning OA emissions. Black carbon particle core sizes typically range from 250–290 nm, while coating thicknesses range from 40–110 nm in air masses less influenced by precipitation. The primary driver of the variability we observe appears to be related to changes at the initial fire source. A key lesson from our study is that the complex nature of the regional aerosol and its drivers precludes aggregating our observations as a function of atmospheric aging due to the many conflating and competing factors present. Our study explores and quantifies key uncertainties in the evolution of biomass burning aerosol at both nearfield and regional scales. Our results suggest that the initial conditions of the fire are the primary driver of carbonaceous aerosol physical and chemical properties over tropical South America, aside from significant oxidation of OA during atmospheric aging. Such findings imply that uncertainties in the magnitude of the aerosol burden and its impact on weather, climate, health and natural ecosystems most likely lie in quantifying emission sources, alongside atmospheric dispersion, transport and removal rather than chemical enhancements in mass.