Rotational and dilational reconstruction in transition metal dichalcogenide moiré bilayers

Madeline Winkle, Isaac M. Craig, Stephen Carr, Medha Dandu, Karen C. Bustillo, Jim Ciston, Colin Ophus, Takashi Taniguchi, Kenji Watanabe, Archana Raja, Sinéad M. Griffin and D. Kwabena Bediako ()
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Madeline Winkle: University of California
Isaac M. Craig: University of California
Stephen Carr: Brown University
Medha Dandu: Lawrence Berkeley National Laboratory
Karen C. Bustillo: Lawrence Berkeley National Laboratory
Jim Ciston: Lawrence Berkeley National Laboratory
Colin Ophus: Lawrence Berkeley National Laboratory
Takashi Taniguchi: National Institute for Materials Science
Kenji Watanabe: National Institute for Materials Science
Archana Raja: Lawrence Berkeley National Laboratory
Sinéad M. Griffin: Lawrence Berkeley National Laboratory
D. Kwabena Bediako: University of California

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Lattice reconstruction and corresponding strain accumulation plays a key role in defining the electronic structure of two-dimensional moiré superlattices, including those of transition metal dichalcogenides (TMDs). Imaging of TMD moirés has so far provided a qualitative understanding of this relaxation process in terms of interlayer stacking energy, while models of the underlying deformation mechanisms have relied on simulations. Here, we use interferometric four-dimensional scanning transmission electron microscopy to quantitatively map the mechanical deformations through which reconstruction occurs in small-angle twisted bilayer MoS2 and WSe2/MoS2 heterobilayers. We provide direct evidence that local rotations govern relaxation for twisted homobilayers, while local dilations are prominent in heterobilayers possessing a sufficiently large lattice mismatch. Encapsulation of the moiré layers in hBN further localizes and enhances these in-plane reconstruction pathways by suppressing out-of-plane corrugation. We also find that extrinsic uniaxial heterostrain, which introduces a lattice constant difference in twisted homobilayers, leads to accumulation and redistribution of reconstruction strain, demonstrating another route to modify the moiré potential.

Date: 2023
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DOI: 10.1038/s41467-023-38504-7

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