Advanced field theoretic simulations of polymer nanocomposites

Jason Koski, University of Pennsylvania


Polymers nanocomposites (PNCs) have emerged as a promising class of materials that can exhibit enhanced mechanical, optical, and electrical properties over polymers or nanoparticles alone. The outstanding issue is that the parameter space associated with PNCs is vast and a global framework for what parameters and processing conditions determine the resulting structure is lacking. Polymer field theory has been established as the primary tool in understanding inhomogeneous polymer systems. Here, we extend the polymer field theory framework to efficiently model PNCs, which we refer to as polymer nanocomposite field theory (PNC-FT). The utility of the PNC-FT method is the ability to efficiently study the thermodynamics and vast parameter space associated with PNCs. The PNC-FT method is developed to efficiently model a wide array of systems: nanospheres, nanorods, grafted nanoparticles with simple (homopolymer) and complex (diblock, mixed, and Janus) grafting architectures. Moreover, a numerical dynamic mean-field theory (DMFT) is presented as an additional tool to capture non-equilibrium behavior in PNC systems. The PNC-FT framework is validated through comparisons with Monte Carlo simulations and by demonstrations of the ability to capture particle correlations, a feature that is not captured in the conventional polymer field theory framework. The PNC-FT method is used to study: the ideal domain spacing of lamellar forming block copolymer nanocomposites, the segregation of homopolymers and nanoparticles to tilt grain boundaries in block copolymer thin films, complex grafted nanoparticles acting as surfactants in a homopolymer blend, and grafted gold nanorods in polymer thin films. The grafted gold nanorod study is done in direct collaboration with experimentalists where we provide an additional systematic study that demonstrates the advantages and disadvantages of: a previously developed hybrid particle-field theory (HPFT), PNC-FT, and DMFT. In investigating this wide range of systems, we demonstrate the efficacy of the PNC-FT and DMFT approaches in developing paramter-structure-property and process-structure-property relationships in PNCs, respectively.

Subject Area

Chemical engineering|Materials science

Recommended Citation

Koski, Jason, "Advanced field theoretic simulations of polymer nanocomposites" (2016). Dissertations available from ProQuest. AAI10190782.