Grains and grain boundaries in single-layer graphene atomic patchwork quilts

The properties of polycrystalline materials are often dominated by the size of their grains and by the atomic structure of their grain boundaries. These effects should be especially pronounced in 2D materials, where even a line defect can divide and disrupt a crystal. These issues take on practical significance in graphene, a hexagonal two-dimensional crystal of carbon atoms; Single-atom-thick graphene sheets can now be produced by chemical vapor deposition on up to meter scales, making their polycrystallinity almost unavoidable. Theoretically, graphene grain boundaries are predicted to have distinct electronic, magnetic, chemical, and mechanical properties which strongly depend on their atomic arrangement. Yet, because of the five-order-of-magnitude size difference between grains and the atoms at grain boundaries, few experiments have fully explored the graphene grain structure. Here, we use a combination of old and new transmission electron microscope techniques to bridge these length scales. Using atomic-resolution imaging, we determine the location and identity of every atom at a grain boundary and find that different grains stitch together predominantly via pentagon-heptagon pairs. We then use diffraction-filtered imaging to rapidly map the location, orientation, and shape of several hundred grains and boundaries, where only a handful have been previously reported. The resulting images reveal an unexpectedly small and intricate patchwork of grains connected by tilt boundaries. By correlating grain imaging with scanned probe measurements, we show that these grain boundaries dramatically weaken the mechanical strength of graphene membranes, but do not measurably alter their electrical properties. These techniques open a new window for studies on the structure, properties, and control of grains and grain boundaries in graphene and other 2D materials.