Data for: Deterministic fabrication of graphene/hexagonal boron nitride moire superlattices

The electronic properties of moire heterostructures depend sensitively on the relative orientation between layers of the stack.
For example, near-magic-angle twisted bilayer graphene (TBG) commonly shows superconductivity, yet a TBG sample with one of the graphene layers rotationally aligned to a hexagonal Boron Nitride (hBN) cladding layer provided the first experimental observation of orbital ferromagnetism. To create samples with aligned graphene/hBN, researchers often align edges of exfoliated flakes that appear straight in optical micrographs. However, graphene or hBN can cleave along either zig-zag or armchair lattice directions, introducing a 30 degree ambiguity in the relative orientation of two flakes. By characterizing the crystal lattice orientation of exfoliated flakes prior to stacking using Raman and second-harmonic generation for graphene and hBN, respectively, we unambiguously align monolayer graphene to hBN at a near-0 degrees, not 30 degrees, relative twist angle. We confirm this alignment by torsional force microscopy (TFM) of the graphene/hBN moire on an open-face stack, and then by cryogenic transport measurements, after full encapsulation with a second, non-aligned hBN layer. This work demonstrates a key step toward systematically exploring the effects of the relative twist angle between dissimilar materials within moire heterostructures.