Topological Winding Number Change and Broken Inversion Symmetry in a Hofstadter's Butterfly

Graphene's quantum Hall features are associated with a π Berry's phase due to its odd topological pseudospin winding number. In nearly aligned graphene-hexagonal BN heterostructures, the lattice and orientation mismatch produce a superlattice potential, yielding secondary Dirac points in graphene's electronic spectrum, and under a magnetic field, a Hofstadter butterfly-like energy spectrum. Here we report an additional π Berry's phase shift when tuning the Fermi level past the secondary Dirac points, originating from a change in topological winding number from odd to even when the Fermi-surface electron orbit begins to enclose the secondary Dirac points. At large hole doping inversion symmetry breaking generates a distinct hexagonal pattern in the longitudinal resistivity versus magnetic field and charge density. Major Hofstadter butterfly features persist up to ∼100 K, demonstrating the robustness of the fractal energy spectrum in these systems.