Glass transition and viscoelastic properties of polymer nanocomposites with integrated interface design

Polymer nanocomposites (PNCs) are important lightweight materials with tunable functionalities that have been widely used in energy, environment, medication, and infrastructure. It has been proposed more than 20 years ago that controlling the interface of PNCs can lead to a rational design of PNCs with desired macroscopic properties. Two decades of active research have not been able to achieve the goal of the precise design of interfaces in PNCs. In this contribution, we combine chemical synthesis and interface design for new types of polymer-nanoparticle hybrids. With a combination of broadband dielectric spectroscopy, differential scanning calorimetry, and rheology, we show the glass transition and viscoelastic properties of the polymer-nanoparticle hybrids can be rationally tuned to the extent not accessible in other types of polymer nanocomposites. These new results could lead to alternative strategies of interface design of polymer nanocomposites for desired macroscopic properties.