Discrete element method model of soot aggregates

Soot aerosols emitted during combustion can affect climate by scattering and absorbing the sunlight. Individual soot particles are fractal aggregates composed of elemental carbon. In the atmosphere, these aggregates acquire coatings by condensation and coagulation, resulting in significant compaction of the aggregates that changes the direct climate forcing of soot. Currently, no models exist to rigorously describe the process of soot restructuring, reducing prediction accuracy of atmospheric aerosol models. We develop a discrete element method contact model to simulate restructuring of fractal soot aggregates, represented as assemblies of spheres joined by cohesion and by sintered necks. The model is parametrized based on atomic force spectroscopy data and is used to simulate soot restructuring, showing that the fraction of necks in aggregates determines the restructuring pathway. Aggregates with fewer necks undergo local compaction, while aggregates with nearly full necking prefer global compaction. Additionally, full compaction occurs within tens of nanoseconds, orders of magnitude faster than the timescale of soot aging through condensation. An important implication is that the rate of condensation determines how many necks are fractured simultaneously, affecting the restructuring pathway, e.g., producing more compact soot at lower condensation rates than at faster condensation rates for comparable amounts of condensate formed on soot.