Cryogenic nano-imaging of second-order moiré superlattices

Second-order superlattices form when moiré superlattices with similar periodicities interfere with each other, leading to larger superlattice periodicities. These crystalline structures are engineered using two-dimensional materials such as graphene and hexagonal boron nitride, and the specific alignment plays a crucial role in facilitating correlation-driven topological phases. Signatures of second-order superlattices have been identified in magnetotransport experiments; however, real-space visualization is still lacking. Here we reveal the second-order superlattice in magic-angle twisted bilayer graphene closely aligned with hexagonal boron nitride through electronic transport measurements and cryogenic nanoscale photovoltage measurements and evidenced by long-range periodic photovoltage modulations. Our results show that even minuscule strain and twist-angle variations as small as 0.01° can lead to drastic changes in the second-order superlattice structure. Our real-space observations, therefore, serve as a ‘magnifying glass’ for strain and twist angle and can elucidate the mechanisms responsible for the breaking of spatial symmetries in twisted bilayer graphene.