Determination of and evidence for non-core-shell structure of particles containing black carbon using the Single-Particle Soot Photometer (SP2)



[1] The large uncertainty associated with black carbon (BC) direct forcing is due, in part, to the dependence of light absorption of BC-containing particles on the position of the BC within the particle. It is predicted that this absorption will be greatest for an idealized core-shell configuration in which the BC is a sphere at the center of the particle whereas much less absorption should be observed for particles in which the BC is located near or on the surface. Such microphysical information on BC-containing particles has previously been provided only by labor-intensive microscopy techniques, thus often requiring that climate modelers make assumptions about the location of the BC within the particle that are based more on mathematical simplicity than physical reality. The present paper describes a novel analysis method that utilizes the temporal behavior of the scattering and incandescence signals from individual particles containing refractory BC (rBC) measured by the Single-Particle Soot Photometer (SP2) to distinguish particles with rBC near the surface from those that have structures more closely resembling the core-shell configuration. This approach permits collection of a high-time-resolution data set of the fraction of rBC-containing particles with rBC near the surface. By application of this method to a plume containing tracers for biomass burning, it was determined that this fraction was greater than 60%. Such a data set will not only provide previously unavailable information to the climate modeling community, allowing greater accuracy in calculating rBC radiative forcing, but also will yield insight into aerosol processes.