In the forthcoming, we refer to structures calculated using atomistic classical force fields (ReaxFF) and band structures calculated at the DFTB level. For validation of the DFTB electronic structure, see the Methods Section and Figures and. with respect to the low-energy 𝑅 ℎ 𝑀 and 𝐻 ℎ ℎ stackings (for the interlayer distance and interlayer energy of the high-symmetry stackings see Table ). Both moiré cells contain 4902 atoms and, thus, 29412 valence electrons. For twisted 𝑅 ℎ 𝑀 BLs (𝜃 → 0°), the moiré pattern transforms to triangular domains, also predominantly of 𝑅 ℎ 𝑀 stacking, separated by so-called strain solitons . In neighboring triangles, the 𝑅 ℎ 𝑀 lattice is inverted, and all domains have the same surface area for a given twist angle. The nodes are formed of high-energy 𝑅 ℎ ℎ stackings. In contrast, when twisting the centrosymmetric 𝐻 ℎ ℎ configuration (𝜃 → 60°), two different domains emerge due to symmetry, namely larger 𝐻 ℎ ℎ domains and smaller 𝐻 ℎ 𝑋 domains, while the nodes have predominantly high-energy 𝐻 ℎ 𝑀 configuration. All lowenergy stacking domains have very similar interlayer distances of 6.03-6.04 Å and relative energies within 2 meV per unit cell (Figure ). The nodes are subject to high-energy stackings with larger interlayer distance of ~6.5 Å, which causes a layer corrugation of ~0.5 Å (Table ). The solitons show an intermediate-energy stacking with an interlayer distance of ~6.14 Å. This domain formation becomes more evident for small twist angles and, thus, large moiré cells. An example is depicted in Figure . The local interlayer distance maps of the structures used in Figures and S7 are shown in Figure .