An important observation from the analyses provided above is that the FAs accumulating at the surface do not do so uniformly; they aggregate into tessellated clusters with unique tilt angles, illustrated by the red and white patches visible in Figure . The clustered lipid patches, which are highly ordered, adopt a lower curvature than would otherwise be expected (Figure ) and are separated by rift-like "rivers" in which the lipids relax into a more disordered phase. This behavior can be attributed to the balance between the high bending modulus of the FA monolayer (i.e., energy required to perturb the equilibrium curvature) and the line tension of the curved particle surface. This phenomenon has been seen in previous laboratory studies of surfactant-coated microdroplets; surfactants accumulate into ordered domains at the interface and break apart into smaller, and presumably more planar, domains as the curvature of the interface increases. FA raft curvature increases with increasing chemical complexity, suggesting that the introduced macromolecules contribute to lowering the bending modulus of the monolayer. In the simple systems, the only perturbation to the rigid FA monolayers is BCL, which preferentially embeds between, rather than into, the FA rafts. In the more complex systems, the surfactant monolayers are perturbed by additional chemical species such as LPS, which increases interfacial heterogeneity lends greater flexibility to the monolayers (Figure ). The Lipid A region of LPS preferentially adsorbs to the surface at the rivers but is still able to insert into the ordered FA patches, likely due to the ability of FA-like alkyl chains on Lipid A to align with the monolayer. This behavior has similarly been observed in previous studies of surfactants. BCL and LPS are both observed at the aerosol interface and exhibit dramatic variations in interfacial morphology. To computationally evaluate the surface exposure of these two macromolecules, Figures show LPS and BCL colored by frequency of atmosphere exposure, which highlights the most surface active regions of each molecule. To corroborate our findings experimentally, we conducted Brewster angle microscopy ) appears to largely disrupt the fatty acid monolayers, as expected and observed previously. However, it also appears to aggregate, forming holes in the monolayer with little to no organized fatty acid density. We hypothesize that the tendency for the lipases to stick together to form clusters accounts for the holes in the monolayer surface found in BAM images. To this end, we analyzed the frequency of finding BCL-BCL aggregates in our simulations and discovered a variety of aggregation postures. Figure shows a selection of BCL-BCL conformations. It is possible that BCL aggregates together and sinks into the aqueous phase, having less affinity for the surface as a cluster. Interactions with FAs binding to exposed hydrophobic regions on the BCL surfaces may also contribute to lowered FA density in these regions, leading to the patchwork formations seen in Figure . LPS, on the other hand (Figure ), aggregates at the surface to form river-like regions of high and low organic content. The behavior seen here, although describing a phenomenon at a much larger scale than our simulations, is consistent with our computational observations. It is unclear, however, what the orientation of the LPS is at the interface. Our simulations suggest that while the lipid tail is much more surface active, nearly the entire LPS molecule maintains some level of surface activity with regions of the sugar chain further from the lipid tail having greater atmosphere exposure than those closer (Figure ). The Lipid A region can insert directly into and contribute to the bright regions with high FA density, while the saccharide headgroup can also adsorb to the surface and appear in the darker, river-like regions. Future studies are needed to help elucidate the mechanisms reported here.