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Characterization of organic residues of size‐resolved fog droplets and their atmospheric implications
Author(s) -
Chakraborty Abhishek,
Ervens Barbara,
Gupta Tarun,
Tripathi Sachchida N.
Publication year - 2016
Publication title -
journal of geophysical research: atmospheres
Language(s) - English
Resource type - Journals
eISSN - 2169-8996
pISSN - 2169-897X
DOI - 10.1002/2015jd024508
Subject(s) - aerosol , aqueous solution , chemistry , volatility (finance) , environmental chemistry , evaporation , analytical chemistry (journal) , meteorology , organic chemistry , physics , financial economics , economics
Size‐resolved fog water samples were collected in two consecutive winters at Kanpur, a heavily polluted urban area of India. Samples were analyzed by an aerosol mass spectrometer after drying and directly in other instruments. Residues of fine fog droplets (diameter: 4–16 µm) are found to be more enriched with oxidized (oxygen to carbon ratio, O/C = 0.88) and low volatility organics than residues of coarse (diameter > 22 µm) and medium size (diameter: 16–22 µm) droplets with O / C of 0.68 and 0.74, respectively. These O/C ratios are much higher than those observed for background ambient organic aerosols, indicating efficient oxidation in fog water. Accompanying box model simulations reveal that longer residence times, together with high aqueous OH concentrations in fine droplets, can explain these trends. High aqueous OH concentrations in smaller droplets are caused by their highest surface‐volume ratio and high Fe and Cu concentrations, allowing more uptake of gas phase OH and enhanced Fenton reaction rates, respectively. Although some volatile organic species may have escaped during droplet evaporation, these findings indicate that aqueous processing of dissolved organics varies with droplet size. Therefore, large (regional, global)‐scale models need to consider the variable reaction rates, together with metal‐catalyzed radical formation throughout droplet populations for accurately predicting aqueous secondary organic aerosol formation.