To quantitatively evaluate the distribution of organic material throughout each aerosol, we subdivided each particle into concentric ellipsoids of equal volume, following the methods developed and described by Karadima et al. For the last snapshot of each simulation, we applied a convex hull method to approximate the bounding ellipsoid, then found a best-fit ellipsoidal mesh to describe the surface of the aerosol (see Supporting Information for details). Using the equations for the best fit ellipsoidal mesh, we then calculated the equations representing concentric ellipsoidal shells encompassing equal volumes. Using atom selections in VMD, 120 we extracted the atoms located in each region defined as the surface, the bulk, or the core, and calculated their mass percentages. We then plotted the distribution of material by mass throughout the three regions (Figure ). This analysis shows that the organic material largely distributes to either the surface or the core (SI Movies M3-M4). Additionally, there is little correlation between the distribution of organic material with the addition of chemical complexity. Since the majority of the organic material in our simulations is amphiphilic or partially water-soluble in character, the particles do not exhibit complete aqueous/organic phase separation. Both FAs and LPS contain hydrophobic tails and polar headgroups, and can thus participate in monolayer, micellar, and bilayer aggregation. Glucose, due to its small size and hydroxy groups, is highly soluble and will remain in solution, integrating into the hydrogen bond network of the aqueous phase. Bulky, branched laminarin, although less soluble than glucose, still contains polar hydroxyl groups that lend it partial solubility.