[1] Brown carbon is a ubiquitous and unidentified component of organic aerosol which has recently come into the forefront of atmospheric research. This component is strongly linked to the class of humic-like substances (HULIS) in aerosol whose ultimate origin is still being debated. Using a simplified spectroscopic method the concentrations of brown carbon have been determined in aqueous extracts of fine aerosol collected during the CARBOSOL project. On the basis of the results of 2-year measurements of several aerosol constituents at six European sites, possible sources of brown carbon are inferred. Biomass burning (possibly domestic wood burning) is shown to be a major source of brown carbon in winter. At elevated sites in spring, smoke from agricultural fires may be an additional source. Direct comparison of measured brown carbon concentrations with HULIS determined by an independent method reveals that the two quantities correlate well at low-elevation sites throughout the year. At high-elevation sites the correlation is still high for winter but becomes markedly lower in summer, implying different sources and/or atmospheric sinks of brown carbon and HULIS. The results shed some light on the relationships between atmospheric brown carbon and HULIS, two illdefined and overlapping components of organic aerosol.
Abstract.Organosulfates have recently come into the focus of organic aerosol research as potentially important components of water-soluble secondary organic aerosol (SOA) which now dominate tropospheric fine aerosol. Their presence has been confirmed by the identification of sulfate esters of abundant biogenic carbonyl compounds in both smog chamber and continental aerosol. However, none of the studies have been able to determine the mass contribution of organosulfates to SOA.In this paper, as possibly the very first attempt to quantify organosulfates in ambient aerosol, we inferred the mass concentrations of organosulfates by concurrently determining mass concentrations of total sulfur, sulfate and methanesulfonate in rural fine aerosol using two highly sensitive analytical techniques. Although uncertainties were relatively large, we found that mass concentrations of organosulfates in water-soluble fine aerosol ranged from 0.02 µgS m −3 to 0.09 µgS m −3 yielding a mass contribution of 6-12% to bulk sulfur concentrations (or 6-14% to sulfate concentrations). The inferred size distribution of organosulfates suggested that they possibly form in heterogeneous reactions from semi-volatile carbonyl compounds with subsequent or concurrent condensation of gaseous sulfuric acid producing a refractory organic film on particle surfaces.
Abstract. Organosulfates have recently come into the focus of organic aerosol research as potentially important components of water-soluble secondary organic aerosol (SOA) which now dominate tropospheric fine aerosol. Their presence has been confirmed by the identification of sulfate esters of abundant biogenic carbonyl compounds in both smog chamber and continental aerosol. However, none of the studies have been able to determine the mass contribution of organosulfates to SOA. In this paper, as possibly the very first attempt to quantify organosulfates in ambient aerosol, we inferred the mass concentrations of organosulfates by concurrently determining mass concentrations of total sulfur, sulfate and methanesulfonate in rural fine aerosol using two highly sensitive analytical techniques. Although uncertainties were relatively large, we found that mass concentrations of organosulfates in water-soluble fine aerosol ranged from 0.02 μgS m−3 to 0.09 μgS m−3 yielding a mass contribution of 6–12% to bulk sulfur concentrations (or 6–14% to sulfate concentrations). The inferred size distribution of organosulfates suggested that they possibly form in heterogeneous reactions from semi-volatile carbonyl compounds with subsequent or concurrent condensation of gaseous sulfuric acid producing a refractory organic film on particle surfaces.
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