2D Colloids: Size- and Shape-Controlled 2D Materials at Fluid-Fluid Interfaces.

Advances in synthesis of model 3D colloidal particles with exotic shapes and physical properties have enabled discovery of new 3D colloidal phases not observed in atomic systems, and simulations and quasi-2D studies suggest 2D colloidal systems have an even richer phase behavior. However, a model 2D (one-atom-thick) colloidal system has yet to be experimentally realized because of limitations in solution-phase exfoliation of 2D materials and other 2D particle fabrication technologies. Herein, we use a photolithography-based methodology to fabricate size- and shape-controlled monolayer graphene particles, and then transfer the particles to an air-water interface to study their dynamics and self-assembly in real-time using interference reflection microscopy. Results suggest the graphene particles behave as "hard" 2D colloidal particles, with entropy influencing the self-assembled structures. Additional evidence suggests the stability of the self-assembled structures manifests from the edge-to-edge van der Waals force between 2D particles. We also show graphene discs with diameters up to 50 μm exhibit significant Brownian motion under optical microscopy due to their low mass. This work establishes a facile methodology for creating model experimental systems of colloidal 2D materials, which will have a significant impact on our understanding of fundamental 2D physics. Finally, our results advance our understanding of how physical particle properties affect the interparticle interactions between monolayer 2D materials at fluid-fluid interfaces. This information can be used to guide the development of scalable synthesis techniques (e.g., solution-phase processing) to produce bulk suspensions of 2D materials with desired physical particle properties that can be used as building blocks for creating thin films with desired structures and properties via interfacial film assembly.