A locally ab initio computational framework for arbitrary incommensurate materials interfaces

Abstract

Incommensurate materials interfaces constitute a broad and technologically important class of systems, yet their lack of shared periodicity limits predictive and computationally efficient first-principles electronic-structure methods. Here we introduce a scalable computational framework for constructing locally ab initio electronic Hamiltonians for arbitrary materials interfaces. Our approach exploits the nearsightedness of Wannier Hamiltonian matrix elements, enabling their systematic extrapolation and interpolation across interlayer registries. This strategy yields transferable Hamiltonians that retain first-principles accuracy while bypassing the need for prohibitively large commensurate supercells or Moiré approximations. We validate the framework on quasicrystalline 30° twisted bilayer graphene, reproducing experimentally observed spectral features including mirrored Dirac cones and minigaps at avoided crossings arising from generalized interlayer scattering. We further predict quasiperiodic flat-band states in experimentally accessible doping regimes. By enabling predictive electronic-structure calculations across structurally incommensurate interfaces, this framework establishes a practical route to first-principles exploration of emergent interfacial phenomena.