Atmospheric tar balls: aged primary droplets from biomass burning?

Abstract. Atmospheric tar balls are particles of special morphology and composition that are fairly abundant in the plumes of biomass smoke. These particles form a specific subset of brown carbon (BrC) which has been shown to play a significant role in atmospheric shortwave absorption and, by extension, climate forcing. Here we suggest that tar balls are produced by the direct emission of liquid tar droplets followed by heat transformation upon biomass burning. For the first time in atmospheric chemistry we generated tar-ball particles from liquid tar obtained previously by dry distillation of wood in an all-glass apparatus in the laboratory with the total exclusion of flame processes. The particles were perfectly spherical with a mean optical diameter of 300 nm, refractory, externally mixed, and homogeneous in the contrast of the transmission electron microscopy (TEM) images. They lacked any graphene-like microstructure and exhibited a mean carbon-to-oxygen ratio of 10. All of the observed characteristics of laboratory-generated particles were very similar to those reported for atmospheric tar-ball particles in the literature, strongly supporting our hypothesis regarding the formation mechanism of atmospheric tar-ball particles.