Quantitative control of orientational and positional disorder in nanopatterned arrays of metal-infiltrated block copolymers

Correlated disorder is not uncommon in nature and often possesses unexpectedly unique properties, inspiring scientists to explore disorder as a functional design element. However, the controlled realization and reproduction of disordered nanostructures remain experimentally challenging, with the concept of “disorder” itself implying its multifaceted nature. Here, we present a methodology to tune structural disorder using metal-infiltrated block copolymers. Starting from a single-grain hexagonal lattice formed by sphere-forming block copolymer thin films, we intentionally introduce and modulate disorder by controlling annealing temperatures and the type of incorporated metals. We establish a robust analytical framework to quantify the order/disorder parameters, providing a clear yet precise assessment of structural irregularity. Supported by molecular dynamics simulations that reveal the mechanisms of disorder formation, we demonstrate a comprehensive dispersion spectrum of nanoparticles—ranging from highly ordered to disordered states. Supported by phononic bandgap calculations, we show that this continuum can serve as a platform for the controlled engineering of disordered wave-manipulating systems. Structural disorder can lead to fascinating functions, but controlling its extent poses an experimental challenge. Here, the authors develop a method to systematically tune and quantify nanoscale disorder in metal-infiltrated block copolymers.