[42] were used. A converged Monkhorst-Pack k-point grid of 2 × 2 × 1 was applied for systems with 2.28°≤ 𝜃 ≤ 6.01° as well as 53.99°≤ 𝜃 ≤ 57.72°, while for systems with 𝜃 < 2.28° and 𝜃 > 57.72° a 1× 1 × 1 grid was applied. A vacuum of 20 Å normal to the bilayer plane was added to avoid any interactions caused by periodic images. The electronic band structures of the high-symmetry bilayer stackings and exemplary tBL systems with 𝜃 =3.89° and 𝜃 =56.11° were compared at both DFT/PBE and DFTB levels of theory, as shown in Figures and. The band gaps, band dispersions, and formation of Dirac bands were all found to be in good agreement, which supports the choice of the DFTB method for further investigations of systems with large unit cells.