Moiré Superlattice Structure of Pleated Trilayer Graphene Imaged by 4D Scanning Transmission Electron Microscopy

Moiré superlattices in graphene arise from rotational twists in stacked 2D layers, leading to specific band structures, charge density and interlayer electron and excitonic interactions. The periodicities in bilayer graphene moiré lattices are given by a simple moiré basis vector that describes periodic oscillations in atomic density. The addition of a third layer to form trilayer graphene generates a moiré lattice comprised of multiple harmonics that do not occur in bilayer systems, leading to nontrivial crystal symmetries. Here, we use atomic resolution 4D-scanning transmission electron microscopy to study atomic structure in bilayer and trilayer graphene moiré superlattices and use 4D-STEM to map the electric fields to show subtle variations in the long-range moiré patterns. We show that monolayer graphene folded into an S-bend graphene pleat produces trilayer moiré superlattices with both small (<2°) and larger twist angles (7-30°). Annular in-plane electric field concentrations are detected in high angle bilayers due to overlapping rotated graphene hexagons in each layer. The presence of a third low angle twisted layer in S-bend trilayer graphene, introduces a long-range modulation of the atomic structure so that no real space unit cell is detected. By directly imaging trilayer moiré harmonics that span from picoscale to nanoscale using 4D-STEM, we gain insights into the complex spatial distributions of atomic density and electric fields in trilayer twisted layered materials.