To track the evolution of aerosol shape, we quantified the degree of asphericity, 𝜙, and the relative shape anisotropy parameter, 𝜅 2 , which can be derived from the radius of gyration tensors. As the aerosols evolved, their initial spherical shape often deformed into an ellipsoid which can be characterized using the asphericity term. This term is zero when the particle is a perfect sphere and increases as the shape evolves away from sphericity. In a complementary analysis, 𝜅 2 was used to describe the symmetry of the particle. For rod-like symmetry, 𝜅 2 approaches 1, where all atoms lie along a line, while a value of 0 indicates that the particle has a higher degree of symmetry, such as that of a perfect tetrahedron or sphere. The evolution of 𝜙 and 𝜅 2 for each replicate of each aerosol system is plotted over time in Figure . This analysis of aerosol shape was based on that developed by Karadima et al. A detailed description of the calculations and derivations used here is given in the Supporting Information.