The effects of atmospheric processing on soot particle morphology were studied in the laboratory using the Differential Mobility Analyzer-Aerosol Particle Mass Analyzer (DMA-APM) and the DMA-DMA (Tandem DMA) techniques. To simulate atmospheric processing, combustion soot agglomerates were altered by sulphuric acid vapor condensation, relative humidity (RH) cycling, and evaporation of the sulphuric acid and water by heating. Primary investigated properties were particle mobility size and mass. Secondary properties, derived from these, include effective density, fractal dimension, dynamic shape factor, and the mass fraction of condensed material. A transformation of the soot particles to more compact forms occurs as sulphuric acid and water condense onto fresh soot. The particle mass increases and initially the mobility diameter decreases, indicating restructuring of the soot core, likely due to surface tension forces. For a given soot source and condensing liquid, the degree of compaction depends strongly on the mass (or volume) fraction of condensed material. For water and sulphuric acid condensing on combustion soot, a mass increase of 2-3 times is needed for a transformation to spherical particles. In the limit of spherical particles without voids, the effective density then approaches the inherent material density, the fractal dimension approaches 3 and the dynamic shape factor approaches 1. Our results indicate that under typical atmospheric conditions, soot particles will be fully transformed to spherical droplets on a time scale of several hours. It is expected that the morphology changes and addition of soluble material to soot strongly affect the optical and hygroscopic properties of soot.
Bibliographical noteFunding Information:
This work was supported by the US Department of Energy National Institute for Climate Change Research (DOE-NICCR) and the Robert A. Welch Foundation. RZ acknowledges additional support from the National Natural Science Foundation of China (No. 40728006). JP was supported by a postdoctoral stipend from FORMAS, the Swedish Research Council for Environment, Agricultural Sciences and Spatial Planning. PHM was supported by a NSF Grant (No. BES-0646507). MSc. Mark Emery is acknowledged for help with inversion of the APM data.