Top‐Down Fabrication of Atomic Patterns in Twisted Bilayer Graphene

Abstract Atomic‐scale engineering typically involves bottom‐up approaches, leveraging parameters such as temperature, partial pressures, and chemical affinity to promote spontaneous arrangement of atoms. These parameters are applied globally, resulting in atomic‐scale features scattered probabilistically throughout the material. In a top‐down approach, different regions of the material are exposed to different parameters, resulting in structural changes varying on the scale of the resolution. In this work, the application of global and local parameters is combined in an aberration‐corrected scanning transmission electron microscope (STEM) to demonstrate atomic‐scale precision patterning of atoms in twisted bilayer graphene. The focused electron beam is used to define attachment points for foreign atoms through the controlled ejection of carbon atoms from the graphene lattice. The sample environment is staged with nearby source materials such that the sample temperature can induce migration of the source atoms across the sample surface. Under these conditions, the electron‐beam (top‐down) enables carbon atoms in the graphene to be replaced spontaneously by diffusing adatoms (bottom‐up). Using image‐based feedback control, arbitrary patterns of atoms and atom clusters are attached to the twisted bilayer graphene with limited human interaction. The role of substrate temperature on adatom and vacancy diffusion is explored by first‐principles simulations.