Atmospheric Chemistry and Physics | 2021
Rapid transformation of ambient absorbing aerosols from West African biomass burning
Abstract
Abstract. Seasonal biomass burning (BB) over West Africa is a globally significant source of carbonaceous particles in the atmosphere, which have important\nclimate impacts but are poorly constrained. Here, the evolution of smoke aerosols emitted from flaming-controlled burning of agricultural waste and\nwooded savannah in the Senegal region was characterized over a timescale of half-day advection from the source during the MOYA-2017 (Methane Observation\nYearly Assessment-2017) aircraft campaign. Plumes from such fire types are rich in black carbon (BC) emissions. Concurrent measurements of chemical\ncomposition, organic aerosol (OA) oxidation state, bulk aerosol size and BC mixing state reveal that emitted BB submicron aerosols changed\ndramatically with time. Various aerosol optical properties (e.g. absorption Ångström exponent – AAE – and mass absorption coefficients\n– MACs) also evolved with ageing. In this study, brown carbon (BrC) was a minor fractional component of the freshly emitted BB aerosols\n(<\u20090.5\u2009h), but the increasing AAE with particle age indicates that BrC formation dominated over any loss process over the first\n∼\u200912\u2009h of plume transport. Using different methods, the fractional contribution of BrC to total aerosol absorption showed an\nincreasing trend with time and was ∼\u200918\u2009%–31\u2009% at the optical wavelength of 405\u2009nm after half-day transport. The generated\nBrC was found to be positively correlated with oxygenated and low-volatility OA, likely from the oxidation of evaporated primary OA and secondary OA\nformation. We found that the evolution of BrC with particle age was different in this region compared with previous BB field studies that mainly\nfocused on emissions from smouldering fires, which have shown a high contribution from BrC at the source and BrC net loss upon ageing. This study\nsuggests an initial stage of BrC absorption enhancement during the evolution of BB smoke. Secondary processing is the dominant contributor to BrC\nproduction in this BB region, in contrast to the primary emission of BrC previously reported in other BB studies. The total aerosol absorption\nnormalized to BC mass (MACmeas-BC) was also enhanced with ageing due to the lensing effect of increasingly thick coatings on BC and the\nabsorption by BrC. The effect of ageing on aerosol absorption, represented by the absorption enhancement (EAbs-MAC), was estimated over\ntimescales of hours. MOYA-2017 provides novel field results. The comparisons between MOYA-2017 and previous field studies imply that the evolution\nof absorbing aerosols (BC and BrC) after emission varies with source combustion conditions. Different treatments of absorbing aerosol properties from\ndifferent types of fires and their downwind evolution should be considered when modelling regional radiative forcing. These observational results\nwill be very important for predicting climate effects of BB aerosol in regions controlled by flaming burning of agricultural waste and savannah-like\nbiomass fuels.\n