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Twist angle between two-dimensional (2D) layers is a critical parameter that determines their interfacial properties of van der Waals heterostructure, such as moiré excitons and interfacial ferroelectricity. To achieve better control over these properties for fundamental studies and various applications, there have been considerable efforts to manipulate the twist angle. Despite rigorous efforts to control the twist angle of stacked two-dimensional (2D) layers, there remains a challenge in perfectly aligning the crystalline orientation due to mechanical limitations and the inevitable formation of incommensurate regions. Here, we report a thermally activated atomic reconstruction of randomly stacked transition metal dichalcogenides (TMDs) multilayers into fully commensurate (FC) heterostructures with zero-twist-angle by encapsulation annealing, regardless of twist angles of as-stacked samples and large lattice mismatches. We also demonstrate the selective formation of R- and H-type FC phases with a seamless lateral junction using chemical-vapor-deposited TMDs. The resulting FC phases exhibit strong photoluminescence (PL) enhancement of the interlayer excitons even at room temperature due to their commensurate structure with aligned momentum coordinates. Our work not only shows a way to fabricate zero-twisted 2D bilayers with R and H-type configurations, but also provides a platform for studying their unexplored properties, such as interlayer excitons, interlayer valley, and interlayer ferroelectrics.

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• In Copyright
  

  This version of the article has been accepted for publication, after peer review (when applicable) and is subject to Springer Nature’s AM terms of use, but is not the Version of Record and does not reflect post-acceptance improvements, or any corrections. The Version of Record is available online at: http://dx.doi.org/10.1038/s41563-023-01690-2

Keyword: Twist angle, Commensurate heterostructures, Interlayer excitons

Date published: 2023-10-12

Publisher: Springer Science and Business Media LLC

Journal:

• Nature Materials (ISSN: 14764660) vol. 22 issue. 12 p. 1463-1469

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Manuscript type: Author's version (Accepted manuscript)

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First published URL: https://doi.org/10.1038/s41563-023-01690-2

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Updated at: 2025-09-01 16:24:24 +0900

Published on MDR: 2025-08-30 08:17:28 +0900