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Polarity governs atomic interaction through two-dimensional materials

Abstract

The transparency of two-dimensional (2D) materials to intermolecular interactions of crystalline materials has been an unresolved topic. Here we report that remote atomic interaction through 2D materials is governed by the binding nature, that is, the polarity of atomic bonds, both in the underlying substrates and in 2D material interlayers. Although the potential field from covalent-bonded materials is screened by a monolayer of graphene, that from ionic-bonded materials is strong enough to penetrate through a few layers of graphene. Such field penetration is substantially attenuated by 2D hexagonal boron nitride, which itself has polarization in its atomic bonds. Based on the control of transparency, modulated by the nature of materials as well as interlayer thickness, various types of single-crystalline materials across the periodic table can be epitaxially grown on 2D material-coated substrates. The epitaxial films can subsequently be released as free-standing membranes, which provides unique opportunities for the heterointegration of arbitrary single-crystalline thin films in functional applications.

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Fig. 1: The remote atomic interaction of GaN and Si through 1 ML graphene.
Fig. 2: Penetration distance of the potential fluctuations from the Si, GaAs and GaN substrates.
Fig. 3: The comparison of energy fluctuation from 2D interlayers (graphene and hBN) and substrates (GaN) for graphene-coated and hBN-coated GaN substrates.
Fig. 4: Comparison of the transparency and seeding properties of hBN and graphene.

Data availability

The data that support the findings of this study are available from the corresponding authors on reasonable request.

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Acknowledgements

This material is based on work supported by the Defense Advanced Research Projects Agency (award no. 027049-00001, J. Gimlett), Energy Efficiency and Renewable Energy in the Department of Energy (award no. DE-EE0008151) and Air Force Research Laboratory (FA9453-18-2-0017, D. Wilt). We thank Masdar Institute/Khalifa University, LG Electronics R&D Center and Amore Pacific for their support on the remote epitaxy program at MIT. We also thank the LAM Research Foundation, Analog Devices, Rocky Mountain Vacuum and the MIT Lincoln Laboratory for the general support. Research at Naval Research Laboratory was supported by the Office of Naval Research. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the US Department of Energy under contract no. DE-AC02-05CH11231. H.L. thanks the National Supercomputer Center in Guangzhou for support on the computational resources. K.Q. is supported by China Scholarship Council. K.C. and Y.N. were supported by ASCENT, one of six centres in JUMP, a Semiconductor Research Corporation program sponsored by DARPA. Y.N. also thanks the Texas Advanced Computing Center (TACC) for providing computation resources. S.S. and A.O. acknowledge partial funding from the hBN study by the French National Research Agency under the GANEX Laboratory of Excellence (Labex) project.

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Contributions

J.K., W.K. and K.Q. conceived the experiments. J.C.G., J.K., H.L. and W.K. design theoretical modelling. J.C.G. and H.L. performed the DFT calculation. K.C. and Y.N. performed the KMC simulation. W.K., K.Q., Y.K., K.L., D.L. and S.-H.B. contributed to the 2D material handling, measurements, and synthesis of Si, Ge, GaAs, GaN and LiF, T.O., R.J.M., Y.Z. and S.R. contributed to GaN synthesis, D.K.G., R.L.M.-W. and K.M.D. contributed to the graphene synthesis, S.S. and A.O. contributed to the hBN synthesis and Y.Y. and Y.S.H. contributed to the LiF synthesis. All the authors contributed to the discussions and analysis of the results regarding the manuscript. J.K. directed the team.

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Correspondence to Jeffrey C. Grossman or Jeehwan Kim.

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Supplementary Figures 1–18, Supplementary References 1–19

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Kong, W., Li, H., Qiao, K. et al. Polarity governs atomic interaction through two-dimensional materials. Nature Mater 17, 999–1004 (2018). https://doi.org/10.1038/s41563-018-0176-4

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