Self-organized twist-heterostructures via aligned van der Waals epitaxy and solid-state transformations

This is the authors' abstract. We don't add key points for this paper.

Vertical van der Waals (vdW) heterostructures of 2D crystals with defined interlayer twist are of interest for band-structure engineering via twist moiré superlattice potentials. To date, twist-heterostructures have been realized by micromechanical stacking. Direct synthesis is hindered by the tendency toward equilibrium stacking without interlayer twist. Here, we demonstrate that growing a 2D crystal with fixed azimuthal alignment to the substrate followed by transformation of this intermediate enables a potentially scalable synthesis of twisted heterostructures. Microscopy during growth of ultrathin orthorhombic SnS on trigonal SnS2 shows that vdW epitaxy yields azimuthal order even for non-isotypic 2D crystals. Excess sulfur drives a spontaneous transformation of the few-layer SnS to SnS2, whose orientation – rotated 30° against the underlying SnS2 crystal – is defined by the SnS intermediate rather than the substrate. Preferential nucleation of additional SnS on such twisted domains repeats the process, promising the realization of complex twisted stacks by bottom-up synthesis.