Tailoring the structure of polymer networks with iniferter-mediated photo-growth

Using dissipative particle dynamics (DPD), we developed a computational approach to capture the photo-controlled radical polymerization (“photo-growth”) of polymer gels containing trithiocarbonate (TTC) groups within the network strands. Using this model, we focused on a “primary gel” and illuminated the sample to activate the TTCs, which then interacted with monomer and cross-linker in the solution. At low TTC concentrations, gels composed of compatible monomers formed two distinct, spatially separated layers. Conversely, at high TTC concentration, gels formed from incompatible components displayed a well-intermixed structure. Hence, in the presence of light, variations in the TTC concentration provide a new approach for controllably tailoring the structure of polymer gels, and thereby tailoring the functionality of the network.