Bottom-up and top-down manipulations for multi-order photonic crystallinity in a graphene-oxide colloid

The recent discovery of structural coloration in aqueous graphene-oxide (GO) dispersions has increased the applicability of carbon-based two-dimensional materials. However, the origin of the photonic band-gap is still poorly understood, and its practical manipulation is still in an early developmental stage. Here, we demonstrate full-color reflection with first-And secondorder Bragg reflections in a GO dispersion, and we use two fundamental approaches to manipulate GO photonic crystals, namely, bottom-up and top-down manipulation by controlling the Debye length and using shear or surface fields, respectively. Nanoscopic tailoring of the electrostatic effective thickness and macroscopic smoothing of the curvature of the GO sheet result in similar modifications of the quality and pitch of the photonic crystallinity. Direct observation of the GO particle alignments reveals excellent electrostatic layer-To-layer packing assembly and rather poor in-layer assembly. These results elucidate the mechanism that governs the nematic nature of GO (rather than its lamellar mesophase) and the origin of its photonic crystalline periodicity and provide new methodologies for exploiting these attractive features in actual applications.