Controlling the Atomic Reconstruction in Twisted MoSe$_2$/WSe$_2$ with a Monolayer hBN Spacer

Abstract

Twisted van der Waals heterobilayers are a promising material platform for studying collective exciton many-body phenomena, but near-aligned structures often exhibit a local, anisotropic atomic reconstruction that compromises lateral homogeneity. The present study describes how atomic-scale rearrangement in adjacent regions of hBN-encapsulated, near-aligned MoSe$_2$/WSe$_2$ heterobilayers is controlled by the presence of a mono- or bilayer hBN spacer between the two monolayers. High-angle annular dark-field STEM directly resolves the atomic alignment in both layers and shows that the spacer suppresses the reconstruction and strongly increases the structural uniformity of the heterobilayers. 4D-STEM quantitatively maps local rotation, dilation, and heterostrain, revealing that the separated regions remain consistent with rigid moiré superlattice simulations, whereas without the spacer the structural parameters have two to three times broader distributions. By suppressing reconstruction, ultrathin hBN spacers therefore provide an effective route to enhance lattice homogeneity in MoSe$_2$/WSe$_2$ heterobilayers targeting collective excitonic and optoelectronic phenomena.