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In conventional ferroelectric materials, polarization is an intrinsic property limited by bulk crystallographic structure and symmetry. Recently, it has been demonstrated that polar order can also be accessed using inherently non-polar van der Waals materials through layer-by-layer assembly into heterostructures, wherein interfacial interactions can generate spontaneous, switchable polarization. Here, we show that deliberate interlayer rotations in multilayer vdW heterostructures modulate both the spatial ordering and switching dynamics of polar domains. The engendered tunability is unparalleled in conventional bulk ferroelectrics or polar bilayers. By means of operando transmission electron microscopy we show how alterations of the relative rotations of three WSe₂ layers produce structural polytypes with distinct arrangements of polar domains with either a global or localized switching response. Furthermore, the presence of uniaxial strain generates structural anisotropy that yields a range of switching behaviors, coercivities, and even tunable biased responses. We also provide evidence of mechanical coupling between the two interfaces of the trilayer, a key consideration for the control of switching dynamics in polar multilayer structures more
broadly.

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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/s41565-024-01642-0

Keyword: van der Waals heterostructures, Interlayer rotation, Polarization

Date published: 2024-03-19

Publisher: Springer Science and Business Media LLC

Journal:

• Nature Nanotechnology (ISSN: 17483395) vol. 19 issue. 6 p. 751-757

Funding:

• National Science Foundation DMR-2238196
• U.S. Department of Energy DE-AC02-05CH11231
• Gordon and Betty Moore Foundation 10637
• Canadian Institute for Advanced Research GS21-011
• U.S. Department of Defense FA9550-21-F-0003
• U.S. Department of Energy DE-AC02-05CH11231
• MEXT | Japan Society for the Promotion of Science 20H00354
• MEXT | Japan Society for the Promotion of Science 23H02052
• MEXT | Japan Society for the Promotion of Science 20H00354
• MEXT | Japan Society for the Promotion of Science 23H02052

Manuscript type: Author's version (Accepted manuscript)

MDR DOI:

First published URL: https://doi.org/10.1038/s41565-024-01642-0

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Updated at: 2025-09-05 16:30:25 +0900

Published on MDR: 2025-09-05 16:19:25 +0900