Understanding molecular driving force of self-assembly in highly charged soft materials systems via predictive molecular simulations

The self-assembly of highly charged polymeric systems into ordered nanostructures is of fundamental interest in polymer physics and has practical importance to optimize the ion transport properties for next generation electrolytes. In this work, I'll present our ongoing efforts to understand these highly charged systems through predictive molecular simulations, with a focus on an acid-tethered block copolymer system incorporating ionic liquids, for which experiments showed diverse morphology including low symmetry A15 phase with varying conditions. Our molecular dynamic (MD) simulations enables monitoring the detailed molecular structure and dynamics on the micellar interface between hydrophobic core adn charged ionic domains, which revealed the formation of fascinating, thin ionic shell layers composed of ionic complexes. Importantly, the stability of A15 phase was strongly affected by the interfacial properties and concentration fluctionation of the ions and charged block, resulting in radical changes in the conductivity by an order of magnitude. Our collaborative work provides novel routes to develop advanced polymer electrolyte having tailor-made interfaces.