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Interfacial ferroelectricity in rhombohedral-stacked bilayer transition metal dichalcogenides

Nature Nanotechnology volume 17, pages 367–371 (2022)Cite this article

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Abstract

van der Waals materials have greatly expanded our design space of heterostructures by allowing individual layers to be stacked at non-equilibrium configurations, for example via control of the twist angle. Such heterostructures not only combine characteristics of the individual building blocks, but can also exhibit physical properties absent in the parent compounds through interlayer interactions1. Here we report on a new family of nanometre-thick, two-dimensional (2D) ferroelectric semiconductors, where the individual constituents are well-studied non-ferroelectric monolayer transition metal dichalcogenides (TMDs), namely WSe2, MoSe2, WS2 and MoS2. By stacking two identical monolayer TMDs in parallel, we obtain electrically switchable rhombohedral-stacking configurations, with out-of-plane polarization that is flipped by in-plane sliding motion. Fabricating nearly parallel-stacked bilayers enables the visualization of moiré ferroelectric domains as well as electric field-induced domain wall motion with piezoelectric force microscopy. Furthermore, by using a nearby graphene electronic sensor in a ferroelectric field transistor geometry, we quantify the ferroelectric built-in interlayer potential, in good agreement with first-principles calculations. The new semiconducting ferroelectric properties of these four new TMDs opens up the possibility of studying the interplay between ferroelectricity and their rich electric and optical properties2,3,4,5.

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Fig. 1: Crystal structures and piezoelectric force microscopy of bilayer TMDs.
Fig. 2: Hysteresis in R-stacked bilayer TMD devices.
Fig. 3: Electric field dependence of the polarization.
Fig. 4: Estimation of built-in interlayer potential in R-stacked bilayer TMDs and comparison with theory.

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Data availability

The data shown in the paper are available at Harvard Dataverse42.

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Acknowledgements

We thank S. de la Barrera for fruitful discussions. This research was primarily supported by the US Department of Energy, Office of Science, Basic Energy Sciences, under award number DE-SC0020149 (measurement, data analysis and DFT calculation), by the Center for the Advancement of Topological Semimetals, an Energy Frontier Research Center funded by the US Department of Energy Office of Science, through the Ames Laboratory under contract no. DE-AC02-07CH11358 (device concept and design), by the Army Research Office (nanofabrication development) through grant no. W911NF1810316, and the Gordon and Betty Moore Foundations EPiQS Initiative through grant no. GBMF9463 to P.J-H. This work made use of the Materials Research Science and Engineering Center Shared Experimental Facilities supported by the National Science Foundation (NSF) (grant no. DMR-0819762). This work was performed in part at the Harvard University Center for Nanoscale Systems (CNS), a member of the National Nanotechnology Coordinated Infrastructure Network, which is supported by the National Science Foundation under NSF ECCS award no. 1541959. K.W. and T.T. acknowledge support from the Elemental Strategy Initiative conducted by the MEXT, Japan, grant number JPMXP0112101001, JSPS KAKENHI grant numbers JP20H00354 and the CREST(JPMJCR15F3). K.Y. acknowledges partial support by JSPS Overseas Research Fellowships. Synthesis of WSe2 and MoSe2 was supported by the NSF MRSEC programme through Columbia in the Center for Precision-Assembled Quantum Materials (grant no. DMR-2011738).

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Author notes

  1. These authors contributed equally: Xirui Wang, Kenji Yasuda.

Authors and Affiliations

  1. Department of Physics, Massachusetts Institute of Technology, Cambridge, MA, USA

    Xirui Wang, Kenji Yasuda, Yang Zhang, Liang Fu & Pablo Jarillo-Herrero

  2. Department of Mechanical Engineering, Columbia University, New York, NY, USA

    Song Liu & James Hone

  3. National Institute for Materials Science, Tsukuba, Japan

    Kenji Watanabe & Takashi Taniguchi

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  1. Xirui Wang
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Contributions

K.Y. designed and conceived the project. X.W. and K.Y. fabricated the devices and performed transport measurements. K.Y. performed PFM measurements. Y.Z. and L.F. performed the theoretical calculation. S.L. and J.H. grew the WSe2 and MoSe2 (used in device MoSe2 d1) crystals. K.W. and T.T. grew the BN crystal. X.W., K.Y., Y.Z. and P.J.-H. analysed the data and wrote the paper with the input from all the other authors.

Corresponding authors

Correspondence to Kenji Yasuda or Pablo Jarillo-Herrero.

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Nature Nanotechnology thanks Laura Fumagalli, Jianhua Hao and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Discussion, Tables 1–3 and Figs. 1–24.

Supplementary Video 1

Large-scale lateral PFM images of MoSe2 device p2 under the sequence of gate voltages.

Supplementary Video 2

Large-scale lateral PFM images of MoSe2 device p3 under the sequence of gate voltages.

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Wang, X., Yasuda, K., Zhang, Y. et al. Interfacial ferroelectricity in rhombohedral-stacked bilayer transition metal dichalcogenides. Nat. Nanotechnol. 17, 367–371 (2022). https://doi.org/10.1038/s41565-021-01059-z

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