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Cumulative polarization in conductive interfacial ferroelectrics

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Abstract

Ferroelectricity in atomically thin bilayer structures has been recently predicted1 and measured2,3,4 in two-dimensional materials with hexagonal non-centrosymmetric unit-cells. The crystal symmetry translates lateral shifts between parallel two-dimensional layers to sign changes in their out-of-plane electric polarization, a mechanism termed ‘slide-tronics’4. These observations have been restricted to switching between only two polarization states under low charge carrier densities5,6,7,8,9,10,11,12, limiting the practical application of the revealed phenomena13. To overcome these issues, one should explore the nature of polarization in multi-layered van der Waals stacks, how it is governed by intra- and interlayer charge redistribution and to what extent it survives the addition of mobile charge carriers14. To explore these questions, we conduct surface potential measurements of parallel WSe2 and MoS2 multi-layers with aligned and anti-aligned configurations of the polar interfaces. We find evenly spaced, nearly decoupled potential steps, indicating highly confined interfacial electric fields that provide a means to design multi-state ‘ladder-ferroelectrics’. Furthermore, we find that the internal polarization remains notable on electrostatic doping of mobile charge carrier densities as high as 1013 cm−2, with substantial in-plane conductivity. Using density functional theory calculations, we trace the extra charge redistribution in real and momentum spaces and identify an eventual doping-induced depolarization mechanism.

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Fig. 1: Several polarization states in artificially stacked trilayers.
Fig. 2: Multi-polarization states in naturally grown 3R MoS2.
Fig. 3: Effect of gate bias on the polarization.
Fig. 4: Excess charge distribution calculations for polar bilayers of MoS2 (a,c,e panels) and WSe2 (b,d,f panels).

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Acknowledgements

We thank A. Cerreta (Park Systems) for atomic fluorescence microscopy support and N. Ravid for laboratory support. K.W. and T.T. acknowledge support from JSPS KAKENHI (grant nos. 19H05790, 20H00354 and 21H05233). M.G. has been supported by the Israel Science Foundation and the Directorate for Defense Research and Development grant no. 3427/21 and by the US-Israel Binational Science Foundation grant no. 2020072. L.K. thanks the Aryeh and Mintzi Katzman Professorial Chair and the Helen and Martin Kimmel Award for Innovative Investigation. M.U. acknowledges the financial support of the Israel Science Foundation, grant no. 1141/18, and the binational programme of the National Science Foundation of China and Israel Science Foundation, grant no. 3191/19. O.H. is grateful for the generous financial support of the Israel Science Foundation under grant no. 1586/17, The Ministry of Science and Technology of Israel (project no. 3–16244), the Heineman Chair in Physical Chemistry, and the Naomi Foundation for generous financial support from the the 2017 Kadar Award. M.B.S. acknowledges funding by the European Research Council under the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 852925), and the Israel Science Foundation under grant nos. 1652/18 and 3623/21. O.H. and M.B.S. acknowledge the Centre for Nanoscience and Nanotechnology of Tel Aviv University.

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  1. These authors contributed equally: Swarup Deb, Wei Cao

Authors and Affiliations

  1. School of Physics and Astronomy, Tel Aviv University, Tel Aviv, Israel

    Swarup Deb, Noam Raab, Moshe Goldstein & Moshe Ben Shalom

  2. Department of Physical Chemistry, School of Chemistry, The Raymond and Beverly Sackler Faculty of Exact Sciences and The Sackler Center for Computational Molecular and Materials Science, Tel Aviv University, Tel Aviv, Israel

    Wei Cao, Michael Urbakh & Oded Hod

  3. Research Center for Functional Materials, National Institute for Materials Science, Tsukuba, Japan

    Kenji Watanabe

  4. International Center for Materials Nanoarchitectonics, National Institute for Materials Science, Tsukuba, Japan

    Takashi Taniguchi

  5. Department of Molecular Chemistry and Materials Science, Weizmann Institute of Science, Rehovoth, Israel

    Leeor Kronik

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  1. Swarup Deb
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Contributions

S.D. and N.R. conducted the experiments supervised by M.B.S. W.C. conducted the DFT calculations supervised by L.K., M.U. and O.H. K.W. and T.T. provided the h-BN crystals. S.D., W.C., N.R., M.G., L.K., M.U., O.H. and M.B.S. analysed the data, discussed the results and wrote the manuscript.

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Correspondence to Moshe Ben Shalom.

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Deb, S., Cao, W., Raab, N. et al. Cumulative polarization in conductive interfacial ferroelectrics. Nature 612, 465–469 (2022). https://doi.org/10.1038/s41586-022-05341-5

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