Aged boreal biomass-burning aerosol size distributions from BORTAS 2011

Biomass-burning aerosols contribute to aerosol radiative forcing on the climate system. The magnitude of this effect is partially determined by aerosol size distributions, which are functions of source fire characteristics (e.g. fuel type, MCE) and in-plume microphysical processing. The uncertainties in biomass-burning emission number-size distributions in climate model inventories lead to uncertainties in the CCN (cloud condensation nuclei) concentrations and forcing estimates derived from these models. The BORTAS-B (Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellite) measurement campaign was designed to sample boreal biomass-burning outflow over eastern Canada in the summer of 2011. Using these BORTASB data, we implement plume criteria to isolate the characteristic size distribution of aged biomass-burning emissions (aged similar to 1-2 days) from boreal wildfires in northwestern Ontario. The composite median size distribution yields a single dominant accumulation mode with D-pm = 230 nm (number-median diameter) and sigma = 1.5, which are comparable to literature values of other aged plumes of a similar type. The organic aerosol enhancement ratios (Delta OA / Delta CO) along the path of Flight b622 show values of 0.09-0.17 mu g m(-3) ppbv(-1) (parts per billion by volume) with no significant trend with distance from the source. This lack of enhancement ratio increase/decrease with distance suggests no detectable net OA (organic aerosol) production/evaporation within the aged plume over the sampling period (plume age: 1-2 days), though it does not preclude OA production/loss at earlier stages. A Lagrangian microphysical model was used to determine an estimate of the freshly emitted size distribution corresponding to the BORTAS-B aged size distributions. The model was restricted to coagulation and dilution processes based on the insignificant net OA production/evaporation derived from the Delta OA / Delta CO enhancement ratios. We estimate that the young-plume median diameter was in the range of 59-94 nm with modal widths in the range of 1.7-2.8 (the ranges are due to uncertainty in the entrainment rate). Thus, the size of the freshly emitted particles is relatively unconstrained due to the uncertainties in the plume dilution rates.