Controlled alignment of supermoiré lattice in double-aligned graphene heterostructures

The supermoiré lattice, built by stacking two moiré patterns, provides a platform for creating flat mini-bands and studying electron correlations. An ultimate challenge in assembling a graphene supermoiré lattice is in the deterministic control of its rotational alignment, which is made highly aleatory due to the random nature of the edge chirality and crystal symmetry. Employing the so-called "golden rule of three", here we present an experimental strategy to overcome this challenge and realize the controlled alignment of double-aligned hBN/graphene/hBN supermoiré lattice, where the twist angles between graphene and top/bottom hBN are both close to zero. Remarkably, we find that the crystallographic edge of neighboring graphite can be used to better guide the stacking alignment, as demonstrated by the controlled production of 20 moiré samples with an accuracy better than ~ 0.2°. Finally, we extend our technique to low-angle twisted bilayer graphene and ABC-stacked trilayer graphene, providing a strategy for flat-band engineering in these moiré materials.