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Soot particles are the most strongly light-absorbing particlescommonly found in the atmosphere. They are major contributorsto the radiative budget of the Earth and to the toxicity ofatmospheric pollution. Atmospheric aging of soot may changeits health- and climate-relevant properties by oxidizing theprimary black carbon (BC) or organic particulate matter (OM)which, together with ash, comprise soot. This atmosphericaging, which entails the condensation of secondary particulatematter as well as the oxidation of the primary OM and BCemissions, is currently poorly understood. In this study, atmospheric aging of wood-stove soot aerosolswas simulated in a continuous-flow reactor. The composition offresh and aged soot particles was measured in real time by adual-vaporizer aerosol-particle mass spectrometer (SP-AMS).The dual-vaporizer SP-AMS provided information on the OM and BC componentsof the soot as well as on refractory components internally mixed with BC. By switching theSP-AMS laser vaporizer off and using only the AMS thermal vaporizer (at600 °C), information on the OM component only was obtained.In both modes, OM appeared to be generatedlargely by cellulose and/or hemicellulose pyrolysis and wasonly present in large amounts when new wood was added to thestove.In SP-AMS mode, BC signals otherwise dominated the mass spectrum. Thesesignals consisted of ions related to refractory BC (rBC, C1-5+),oxygenated carbonaceous ions(CO1-2+), potassium (K+), and water(H2O+ and related fragments). TheC4+ : C3+ ratio, but not theC1+ : C3+ ratio, was consistent with theBC-structure trends of Corbin et al. (2015c). TheCO1-2+ signals likely originated from BC surfacegroups: upon aging, both CO+ and CO2+increased relative to C1-3+ whileCO2+ simultaneously increased relative toCO+. Factor analysis (positive matrix factorization) of SP-AMS and AMS data,using a modified error model to address peak-integrationuncertainties, indicated that the surface composition of the BCwas approximately constant across all stages of combustion forboth fresh and aged samples. These results represent the firsttime-resolved measurements of in situ BC surface aging andsuggest that the surface of beech-wood BC may be modelled as asingle chemical species

Black carbon surface oxidation and organic composition of beech-wood soot aerosols