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Abstract. Biomass burning is a major source of trace gases andaerosols that can ultimately impact health, air quality, and climate.Global and regional-scale three-dimensional Eulerian chemical transportmodels (CTMs) use estimates of the primary emissions from fires and canunphysically mix them across large-scale grid boxes, leading to incorrectestimates of the impact of biomass burning events. On the other hand,plume-scale process models allow for explicit simulation and examination ofthe chemical and physical transformations of trace gases and aerosols withinbiomass burning smoke plumes, and they may be used to developparameterizations of this aging process for coarser grid-scale models. Herewe describe the coupled SAM-ASP plume-scale process model, which consists ofcoupling the large-eddy simulation model, the System for AtmosphericModelling (SAM), with the detailed gas and aerosol chemistry model, theAerosol Simulation Program (ASP). We find that the SAM-ASP version 1.0 modelis able to correctly simulate the dilution of CO in a California chaparralsmoke plume, as well as the chemical loss of NOx, HONO, and NH3within the plume, the formation of PAN and O3, the loss of OA, and thechange in the size distribution of aerosols as compared to measurements andprevious single-box model results. The newly coupled model is able tocapture the cross-plume vertical and horizontal concentration gradients asthe fire plume evolves downwind of the emission source. The integration andevaluation of SAM-ASP version 1.0 presented here will support thedevelopment of parameterizations of near-source biomass burning chemistrythat can be used to more accurately simulate biomass burning chemical andphysical transformations of tracegases and aerosols within coarser grid-scale CTMs. 

Abstract. Biomass burning emits vapors and aerosols into the atmosphere thatcan rapidly evolve as smoke plumes travel downwind and dilute, affectingclimate- and health-relevant properties of the smoke. To date, theory hasbeen unable to explain observed variability in smoke evolution. Here, we useobservational data from the Biomass BurningObservation Project (BBOP) field campaign and show that initial smokeorganic aerosol mass concentrations can help predict changes in smokeaerosol aging markers, number concentration, and number mean diameterbetween 40–262 nm. Because initial field measurements of plumes aregenerally >10 min downwind, smaller plumes will have alreadyundergone substantial dilution relative to larger plumes and have lowerconcentrations of smoke species at these observations closest to the fire.The extent to which dilution has occurred prior to the first observation isnot a directly measurable quantity. We show that initial observed plumeconcentrations can serve as a rough indicator of the extent of dilutionprior to the first measurement, which impacts photochemistry, aerosolevaporation, and coagulation. Cores of plumes have higher concentrationsthan edges. By segregating the observed plumes into cores and edges, we findevidence that particle aging, evaporation, and coagulation occurred beforethe first measurement. We further find that on the plume edges, the organicaerosol is more oxygenated, while a marker for primary biomass burningaerosol emissions has decreased in relative abundance compared to the plumecores. Finally, we attempt to decouple the roles of the initialconcentrations and physical age since emission by performing multivariatelinear regression of various aerosol properties (composition, size) on thesetwo factors.