Data for Strong atomic reconstruction in twisted bilayers of highly flexible InSe : machine-learned interatomic potential and continuum model approaches

The amount of deviation from a rigid moiré structure will depend on the elastic properties of the constituent monolayers which for the twisted bilayer - the more flexible the monolayers are, the lower the energy required to deform the layers to maximize the areas with an energetically optimal interlayer arrangement of atoms.

We investigate this atomic reconstruction for twisted bilayers of highly flexible InSe. Results using two methods are demonstrated - first we train a machine-learned interatomic potential (MLIP) to enable fully atomistic relaxations of small-twist-angle large-length-scale moiré supercells while retaining density functional theory (DFT) level accuracy. We find substantial out-of-plane corrugation and in-plane domain formation for a wide range of twist angles and moiré length scales.