Evolution of soot particle morphology and mixing state in the atmosphere
Soot particles (aka black carbon) impact the environment and climate by affecting Earth's radiation balance, cloud microphysics, and atmospheric chemistry. The complex morphology and mixing state of soot particles influence their optical properties and therefore their radiative forcing, the particles' transport, lifecycle, and heterogeneous chemistry. How soot morphology and mixing state alter during transport from the source to remote areas is still not well understood. While aging, soot particles can change shape, oxidize and mix, and become coated by organic and inorganic materials. In this study, we investigate the morphological and mixing state evolution of single soot particles in different stages of their 'life' in the atmosphere. This analysis will include an overview of several samples collected in various locations and atmospheric conditions: 1) particles freshly emitted near freeway on-ramps in Southern Michigan (USA); 2) particles emitted in two biomass burning events in New Mexico (USA), one close to the sampling location and another hundreds of miles away; 3) particles in the urban atmosphere of Mexico City and in the uplifted boundary layer captured on the top of the Pico de Tres Padres Mountain (on the north edge of Mexico City); 4) particles collected in the Sacramento urban area and the Sierra Nevada foothills (CA, USA); 5) particles collected in Detling (UK), and mostly transported from London, and 6) long-range transported particles in the free troposphere and collected at the Pico Mountain Observatory, located near the top of the Pico Volcano in the Azores (Portugal). We analyzed a large number of individual particles using electron microscopy and X-ray spectroscopy followed by image analysis. The projected structural properties of soot particles were characterized using size (maximum length, maximum width, and area equivalent diameter) and shape descriptors (e.g., aspect ratio, roundness, and convexity). The particle mass-fractal dimensions were determined using the ensemble method. The mixing state was analyzed by classifying soot particles based on visual inspection of coating and morphology. Soot particles freshly emitted by anthropogenic sources show less coating and more open chain-like structures; on the other hand biomass burning and long-range transported soot particles appear to be mostly coated and exhibit very compacted shapes. However, soot processing in urban atmospheres results in a complex mixture of coated and uncoated particles with a variety of morphologies and mixing states.
Fall Meeting 2013
Mazzoleni, Claudio; China, Swarup; Sharma, Noopur; Gorkowski, K.; Dubey, M.; Aiken, A. C.; Zaveri, R. A.; Salvadori, Neila; Chakrabarty, R. K.; Moosmuller, H.; Onasch, T. B.; Herndon, S.; Williams, L. R.; Liu, S.; Dzepina, K.; Helmig, D.; Hueber, Jacques; Fialho, Paulo; Mazzoleni, L.; Kumar, S.; Dziobak, M. P.; and Wright, K., "Evolution of soot particle morphology and mixing state in the atmosphere" (2013). Department of Chemistry Publications. 42.