Characterizing multi-scale structure and order in hyperuniform polymer grafted nanoparticle assemblies

The study of order and disorder in materials has been a long standing active area of research, as the degree of order can significantly influence the resulting macroscopic behavior. Hyperuniform structures, a more recently defined class of structures, can result in superior performance for controlling critical properties like toughness and efficient control of electromagnetic and mechanical waves. In polymer grafted nanoparticle composites, this structure and order plays a critical role at multiple scales from particle-polymer interfaces to particle morphology to large scale particle arrangements. Understanding this structure at these scales is critical for understanding the measured macroscopic properties. Here, we tailor the synthesis and assembly of polymer grafted nanoparticle thin films to achieve both ordered and disordered hyperuniform arrangements though tailoring the PGN architecture and the processing conditions influencing the large scale self assembly. We study systems of bimodal spherical systems, and assess the degree of orientational and translational disorder through metrics introduced to characterize hyperuniform structures and jammed particle packings. Finally, these structural and processing connections are connected to static and dynamic mechanical properties. This multi-scale process-structure-property understanding will influence the further design of materials and structures for a variety of applications and environments.