Large-Volume Self-Organization of Polymer/Nanoparticle Hybrids with Millimeter-Scale Grain Sizes Using Brush Block Copolymers

We report that an exceptionally large volume of highly ordered arrays (single grains) on the order of millimeters in scale can be rapidly created through a unique innate guiding mechanism of brush block copolymers (BBCPs). The grain volume is over 109 times larger than that of typical self-assembled linear BCPs (LBCPs). The use of strong interactions between nanoparticles (NPs) and BBCPs enables high loadings of functional materials, up to 76 wt % (46 vol %) in the target domain, while maintaining excellent long-range order. Overall, this work provides a simple method to precisely control the spatial orientation of functionalities at nanometer length scales over macroscopic volumes, thereby enabling the production of hybrid materials for many important applications.