Michael Cai Wang1 Wayne Lin1 Matthew Thomas Gole1 Juyoung Leem1 Catherine Murphy1 SungWoo Nam1

1, University of Illinois-Urbana-Champaign, Urbana, Illinois, United States

The deterministic confluence of organized 0D/1D plasmonic nanoparticles (NPs) with atomically-thin 2D materials can lead to novel and tunable near-field effects such as plasmonic/exciton coupling in 0D/1D NPs and 2D semiconductors. However, current top-down strategies to fabricate desired nanoscale resonant architectures based on lithography and metal deposition are limited in their spatial resolution, material quality, and flexibility in morphological configurations for both the resonant nanostructures and the substrate. In contrast, colloidal preparations of plasmonic nanoparticles are extremely versatile and highly scalable, which couple directly to the deterministic surface morphologies formed via deformed atomically-thin 2D materials serving as ideal templates for self-assembly of such 0D/1D NPs. Here, we present a generalized method to self-organize a variety of high quality, colloidally-prepared 0D/1D gold NPs of various geometries and surface chemistries onto deterministically deformed graphene and transition metal chalcogenide (TMDC) monolayers. This is achieved via nanoscale convective self-assembly of 0D/1D NPs onto large-scale, heterogeneously strained, deformed 2D materials templates formed via strain induced mechanical surface instabilities (i.e., buckles, wrinkles, creases, etc.). By controlling simple material parameters, we design deformed 2D materials templates with characteristic features spanning a few dozens of nanometers to tens of microns. This allows independent control over the various factors enabling such versatile assembly (morphology, coverage, ordering) including nanoparticle size, concentration, aspect ratio, surface and solvent chemistry, in addition to the conjugate properties in the deformed 2D material template and supporting substrate (isotropy, periodicity, amplitude, surface energy). By optimizing the various material properties, NPs as small as 15nm can be readily self-assembled up to inch scale into well-organized, massively-parallel, sub-100nm single-file arrays onto deterministically deformed monolayer 2D materials. This development represents a first in realizing self-assembly with mixed-dimensionality deformed nanoscale materials and enables not only new tools to study emergent coupled phenomena in mixed low-dimensional heterogeneous systems but also as a general strategy to realize self-assembly based nanomanufacturing of novel low-dimensional material architectures.