Abstract
While the formation pathways and thermodynamic properties of inorganic species (e.g., sulphate) in atmospheric aerosols are well understood, many more uncertainties exist about organics. In the present study we present oxidation pathways of organic gas phase species that lead to low volatility organic compounds (C2‐C6 dicarboxylic acids, pyruvic acid) in both the aqueous and gas phases. This mechanism is implemented in a cloud parcel model initialized with pure (NH4)2SO4 particles in 10 discrete sizes. Under clean continental conditions a few cloud processing cycles produce a total organic mass addition of ∼150 ng m−3. Individual resuspended aerosol size classes contain significant organic fractions, sometimes higher than 50%. These are likely upper bound estimates of organic mass production. In a polluted, i.e., SO2‐rich scenario, about 400 ng m−3 organic material is produced after about eight cloud cycles. Since the initial conditions in this latter case favor significant production of sulphate, the organic fraction of the aerosol mass after cloud processing represents a much lower percentage of the total aerosol mass. Oxalic, glutaric, adipic, and pyruvic acids are the main contributors to the organic fraction in both cases. In agreement with observations, the oxalate fraction in processed particles exceeds the fractions of other dicarboxylic acids since it represents an end product in the oxidation of several organic gas phase species. The study suggests that cloud processing may act as a significant source of small dicarboxylic acids, some fraction of which can be retained in the aerosol phase upon drop evaporation.
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