Aerosol morphology is a critical driver of many atmospheric properties; particle surfaces mediate interactions with gases and sunlight, while the organization of the aerosol interior regulates the absorption and diffusion of small molecules which can control phase state and water uptake. The current understanding of aerosol morphology is derived from experimental observation. Organic aerosols adopt a variety of morphologies, including the common core-shell morphology, in which organic materials phase separate to the aerosol surface to form a thick coating around a salty aqueous core. Other phase separated morphologies besides core-shell have been observed for model systems (Figure ) and depend on particle size, O:C ratio of the organic species, and/or organic : inorganic mass ratio. However, observations using singleparticle analysis methods can be compromised by a variety of factors including the aerosol generation mechanism, sample storage, and analysis method. Additionally, all microscopy based techniques such as atomic force microscopy (AFM), scanning electron microscopy (SEM), and cryogenic transmission electron microscopy (cryo-TEM), while valuable, require the deposition of aerosols onto a substrate which alters particle shape and surface area, compromising the structural integrity of the particle. Techniques such as microfluidics and aerosol optical tweezers (AOT) are similarly limited in their size resolution, aerosol generation methods, and for AOT, ability to investigate non-spherical particles within a single laser beam trap. Molecular dynamics (MD) simulations (aka computational microscopy) provide an effective alternative to conventional experimental techniques and have been used to interrogate a variety of properties of nanoscale aerosols, including water condensation, 52-58 atmospheric gas uptake, coalescence, 60 and phase state. A majority of these MD studies are related to natural or anthropogenic volatile organic carbon and investigate small aerosol clusters containing low molecular-weight mono-and dicarboxylic acids. Studies of marine aerosols to date have approximated SSA by combining medium-chain fatty acids or free amino acids with saltwater clusters. 55, A central limitation to all MD studies is balancing system size and complexity with simulation length; the simulation of large, complex aerosols for statistically significant timescales is limited by availability of largescale (leadership class) computational resources and scalability of the MD codes. Thus, aerosol models studied have largely contained simple binary or ternary mixtures on the order of <100 Å in diameter and simulated for a duration on the order of <100 ns, which may limit statistically rigorous sampling. Nevertheless, simulations have supported experimental evidence that insoluble organics fully phase separate into a core-shell or partially-engulfed morphology, albeit with short timescales, small system sizes, and a marked lack of organic complexity.