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Three-dimensional nonlinear optical materials from twisted two-dimensional van der Waals interfaces

Nature Photonics volume 18, pages 91–98 (2024)Cite this article

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Abstract

To enable new nonlinear responses, metamaterials are created by organizing structural units (meta-atoms), which are typically on the scale of about a hundred nanometres. However, truly altering the atomic symmetry and enabling new nonlinear responses requires control at the atomic scale, down to a few ångströms. Here we report three-dimensional nonlinear optical materials realized by the precise control and twist of individual two-dimensional van der Waals interfaces. Specifically, new nonlinear crystals are achieved by adding pseudo-screw symmetries to a multiple of four-layer WS2 stacks (for example, four layer, eight layer and so on). Nonlinear susceptibility and circular selectivity of the resulting three-dimensional crystals are fundamentally different from natural WS2, demonstrating a microscopic analogue to the fabrication of metamaterials with unique optical properties. Furthermore, we show that the magnitude of the newly enabled nonlinearity is enhanced by controlling the number of interfaces and the excitation wavelength. Our findings suggest a new approach to redesign the intrinsic nonlinearity in artificial atomic configurations, scalable from a few-nanometre-thick unit cells to bulk materials.

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Fig. 1: Redesigned second-order susceptibility in a twisted 3D crystal.
Fig. 2: Interfacial nonlinear susceptibility in twisted bilayer WS2.
Fig. 3: Scalability of interfacial nonlinear susceptibility in twisted trilayer WS2 stacks.
Fig. 4: Scalable nonlinear optical material.
Fig. 5: Enhanced nonlinear susceptibility by exciton resonances.
Fig. 6: Nonlinear circular selectivity enabled by a four-fold screw symmetry.

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The data in the Article are available from the corresponding author upon reasonable request. Source data are provided with this paper.

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Acknowledgements

This work was partly supported by the National Science Foundation through the University of Pennsylvania Materials Research Science and Engineering Center DMR-1720530 (B.K.), the US Office of Naval Research (ONR) through grant N00014-20-1-2325 on Robust Photonic Materials with High-Order Topological Protection (B.Z., B.K., J.J., Z.W., L.H. and T.C.) and grant N00014-21-1-2703 (B.Z., B.K., J.J., Z.W., L.H. and T.C.) and the Sloan Foundation (B.Z.). Work by E.J.M. is supported by the Department of Energy under grant DE-FG02-84ER45118. T.C. acknowledges the support of a research grant (project no. 42106) from Villum Fonden.

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Authors and Affiliations

  1. Department of Physics and Astronomy, University of Pennsylvania, Philadelphia, PA, USA

    Bumho Kim, Jicheng Jin, Zhi Wang, Li He, Eugene J. Mele & Bo Zhen

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

    Thomas Christensen

  3. Department of Electrical and Photonics Engineering, Technical University of Denmark, Kgs. Lyngby, Denmark

    Thomas Christensen

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Contributions

B.Z. and B.K. conceived the project. B.K. and Z.W. fabricated the twisted stacks. B.K. performed the SHG measurements assisted by J.J. and L.H. B.K. and T.C. performed the symmetry analysis. B.Z., E.J.M. and B.K. discussed and interpreted the results. B.Z. and B.K. wrote the paper with input from all authors. All authors discussed the results.

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Correspondence to Bo Zhen.

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Nature Photonics thanks Wen-Hao Chang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Kim, B., Jin, J., Wang, Z. et al. Three-dimensional nonlinear optical materials from twisted two-dimensional van der Waals interfaces. Nat. Photon. 18, 91–98 (2024). https://doi.org/10.1038/s41566-023-01318-6

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