Self-assembled disordered hyperuniformity in polymer-grafted nanoparticle thin films

The control of microstructural order and disorder in materials strongly influences macroscopic properties. In recent decades, disordered hyperuniform (DHU) structures, characterized by an anomalous suppression of density fluctuations at large length scales, have generated significant interest for their ability to control mechanical and electromagnetic waves, exhibiting photonic and phononic band gaps and potential for enhanced toughness. In polymer-grafted nanoparticle (PGN) composites, microstructure is influenced by processing parameters at multiple length scales, from PGN core size and polymer chain length to the thin film formation process. We tailor the synthesis and self-assembly of thin films by controlling size distributions of PGNs, demonstrating potential for scalable, self-assembled DHU at nm length scales. By varying a range of parameters in the thin-film formation process, we can control large-scale self-assembly of the particle microstructure, which we characterize via TEM to assess hyperuniformity and orientational disorder within the system, and further examine via Brillouin light scattering. This multiscale process-structure-property understanding can provide a framework for scalable design of materials for optical property control and thermal management.