Aerosol size distribution changes in FIREX-AQ biomass burning plumes: the impact of plume concentration on coagulation and OA condensation/evaporation

The evolution of organic aerosol (OA) and aerosol size distributions within smoke plumes is uncertain due to the variability in rates of coagulation and OA condensation/evaporation between different smoke plumes and at different locations within a single plume. We use aircraft data from the FIREX-AQ campaign to evaluate differences in evolving aerosol size distributions, OA, and oxygen to carbon ratios (O : C) between and within smoke plumes during the first several hours of aging as a function of smoke concentration. The observations show that the median particle diameter increases faster in smoke of a higher initial OA concentration (> 1000 mu gm(-3)), with diameter growth of over 100 nm in 8 h - despite generally having a net decrease in OA enhancement ratios - than smoke of a lower initial OA concentration (< 100 mu gm(-3)), which had net increases in OA. Observations of OA and O : C suggest that evaporation and/or secondary OA formation was greater in less concentrated smoke prior to the first measurement (5-57 min after emission). We simulate the size changes due to coagulation and dilution and adjust for OA condensation/evaporation based on the observed changes in OA. We found that coagulation explains the majority of the diameter growth, with OA evaporation/condensation having a relatively minor impact. We found that mixing between the core and edges of the plume generally occurred on timescales of hours, slow enough to maintain differences in aging between core and edge but too fast to ignore the role of mixing for most of our cases.