Atomic reconstruction in twisted bilayers of transition metal dichalcogenides

TL;DR

This study reveals how twisted bilayers of transition metal dichalcogenides undergo atomic reconstruction into distinct stacking domains, significantly affecting their electronic properties and revealing new metastable phases.

Contribution

It combines atomic resolution microscopy and multiscale modeling to uncover the atomic reconstruction and domain formation in twisted TMD bilayers, highlighting new electronic and structural phenomena.

Findings

Reconstruction into energetically favorable stacking domains occurs at small twist angles.

Distinct electronic properties are observed in 3R and 2H stacking domains.

Discovery of a metastable phase with a kagome-like pattern at around 1° twist angle.

Abstract

Van der Waals heterostructures form a massive interdisciplinary research field, fueled by the rich material science opportunities presented by layer assembly of artificial solids with controlled composition, order and relative rotation of adjacent atomic planes. Here we use atomic resolution transmission electron microscopy and multiscale modeling to show that the lattice of MoS$_2$ and WS$_2$ bilayers twisted to a small angle, $\theta<3^{\circ}$, reconstructs into energetically favorable stacking domains separated by a network of stacking faults. For crystal alignments close to 3R stacking, a tessellated pattern of mirror reflected triangular 3R domains emerges, separated by a network of partial dislocations which persist to the smallest twist angles. Scanning tunneling measurements show that the electronic properties of those 3R domains appear qualitatively different from 2H TMDs, featuring layer-polarized conduction band states caused by lack of both inversion and mirror symmetry. In contrast, for alignments close to 2H stacking, stable 2H domains dominate, with nuclei of an earlier unnoticed metastable phase limited to $\sim$ 5nm in size. This appears as a kagome-like pattern at $\theta\sim 1^{\circ}$, transitioning at $\theta\rightarrow 0$ to a hexagonal array of screw dislocations separating large-area 2H domains.