Coarse-graining to create minimalist models for dynamic, end-linked star-polymer networks

Abstract

Although minimalist models for patchy attractive particles have revealed powerful design rules for how particle valence directs colloidal assembly, less work has focused on comparably simple models of reversible, network-forming star polymers. Here, we use relative-entropy coarse-graining and simulation results from finer-resolution bead--spring star polymers to generate 5-bead models of dynamic, end-associating four-armed poly(ethylene glycol) macromers. Our results comparing structural correlations, network connectivity, and phase behavior of the coarse- and fine-grained models provide insight into how the accuracy and transferability of the coarse-grained models depend on the state point chosen for coarse-graining. The results also reveal intrinsic trade-offs between reducing degrees of freedom and expanding the range of effective interactions in coarse-graining that impact the total number of pairwise interactions in the resulting model, with implications for its computational efficiency.

25 pages, 7 figures, 1 table