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Van der Waals quaternary oxides for tunable low-loss anisotropic polaritonics

Nature Nanotechnology (2024)Cite this article

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Abstract

The discovery of ultraconfined polaritons with extreme anisotropy in a number of van der Waals (vdW) materials has unlocked new prospects for nanophotonic and optoelectronic applications. However, the range of suitable materials for specific applications remains limited. Here we introduce tellurite molybdenum quaternary oxides—which possess non-centrosymmetric crystal structures and extraordinary nonlinear optical properties—as a highly promising vdW family of materials for tunable low-loss anisotropic polaritonics. By employing chemical flux growth and exfoliation techniques, we successfully fabricate high-quality vdW layers of various compounds, including MgTeMoO6, ZnTeMoO6, MnTeMoO6 and CdTeMoO6. We show that these quaternary vdW oxides possess two distinct types of in-plane anisotropic polaritons: slab-confined and edge-confined modes. By leveraging metal cation substitutions, we establish a systematic strategy to finely tune the in-plane polariton propagation, resulting in the selective emergence of circular, elliptical or hyperbolic polariton dispersion, accompanied by ultraslow group velocities (0.0003c) and long lifetimes (5 ps). Moreover, Reststrahlen bands of these quaternary oxides naturally overlap that of α-MoO3, providing opportunities for integration. As an example, we demonstrate that combining α-MoO3 (an in-plane hyperbolic material) with CdTeMoO6 (an in-plane isotropic material) in a heterostructure facilitates collimated, diffractionless polariton propagation. Quaternary oxides expand the family of anisotropic vdW polaritons considerably, and with it, the range of nanophotonics applications that can be envisioned.

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Fig. 1: Optical properties of vdW quaternary oxides.
Fig. 2: Observation of in-plane anisotropic edge polaritons.
Fig. 3: Tailoring polariton responses by atomic substitution.
Fig. 4: Diffractionless nanolight canalization by the heterostructure without twist.

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Acknowledgements

We acknowledge support from Z. Dai for Raman measurements and the efforts of Q. Ou and G. Si in exploring the material fabrication. P.L. acknowledges support from the National Natural Science Foundation of China (grant number 62075070) and the National Key Research and Development Program of China (grant number 2021YFA1201500), the Hubei Provincial Natural Science Foundation of China (grant number 2022CFA053) and the Innovation Fund of WNLO. S.Z. acknowledges support from the National Natural Science Foundation of China (grant numbers 22122507, 22193042, 21833010). R.C. acknowledges support from the China Postdoctoral Science Foundation (2021M701298).

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Author notes

  1. These authors contributed equally: Tian Sun, Runkun Chen.

Authors and Affiliations

  1. Wuhan National Laboratory for Optoelectronics and School of Optical and Electronic Information, Huazhong University of Science and Technology, Wuhan, China

    Tian Sun, Weiliang Ma, Qizhi Yan, Xinliang Zhang & Peining Li

  2. Optics Valley Laboratory, Wuhan, China

    Tian Sun, Weiliang Ma, Qizhi Yan, Xinliang Zhang & Peining Li

  3. State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, China

    Runkun Chen, Han Wang, Junhua Luo & Sangen Zhao

  4. Xidian University, Xi’an, China

    Xinliang Zhang

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Contributions

P.L. and S.Z. conceived the study. T.S. fabricated the samples and performed the s-SNOM measurements with the help of W.M. R.C. and T.S. carried out the fitting of the permittivity of the materials. H.W. synthesized the materials with the help of S.Z. T.S., R.C. and W.M. performed the simulations. T.S. and R.C. carried out the far-field experiments. Q.Y. performed the calculation of the phonon band structures. P.L., S.Z., X.Z. and J.L. coordinated and supervised the work. T.S. and P.L. wrote the paper with input from all co-authors. All authors read and approved the final paper.

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Correspondence to Sangen Zhao or Peining Li.

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Sun, T., Chen, R., Ma, W. et al. Van der Waals quaternary oxides for tunable low-loss anisotropic polaritonics. Nat. Nanotechnol. (2024). https://doi.org/10.1038/s41565-024-01628-y

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