Orbital Angular Momentum from Self-Assembled Concentric Nanoparticle Rings

Ring-shaped nanostructures can focus, filter, and manipulate electromagnetic waves, but are challenging to incorporate into devices using standard nanofabrication techniques. Directed self-assembly (DSA) of block copolymers (BCPs) on lithographically patterned templates has successfully been used to fabricate concentric rings and spirals as etching masks. However, this method is limited by BCP phase behavior and material selection. Here, a straightforward approach to generate ring-shaped nanoparticle assemblies in thin films of supramolecular nanocomposites is demonstrated. DSA is used to guide the formation of concentric rings with radii spanning 150-1150 nm and ring widths spanning 30-60 nm. When plasmonic nanoparticles are used, ring nanodevice arrays can be fabricated in one step, and the completed devices produce high-quality orbital angular momentum (OAM). Nanocomposite DSA simplifies and streamlines nanofabrication by producing metal structures without etching or deposition steps; it also introduces interparticle coupling as a new design axis. Detailed analysis of the nanoparticle ring assemblies confirms that the supramolecular system self-regulates the spatial distribution of its components, and thus exhibits a degree of flexibility absent in DSA of BCPs alone, where structures are determined by polymer-pattern incommensurability. The present studies also provide guidelines for developing self-regulating DSA as an alternative to incommensurability-driven methods.