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A solution-processable natural crystal with giant optical anisotropy for efficient manipulation of light polarization

Abstract

Optical anisotropy, a spatially asymmetric light–matter interaction that manifests itself as birefringence and dichroism, is paramount for manipulating light polarization in modern optics. So far, various natural birefringent crystals are widely used, but their birefringence is limited to <0.3. Here we demonstrate a solution-processable natural crystal C3H8N6I6·3H2O with giant birefringence up to 2.8 within the visible to infrared spectral region. Combining critical point analysis and the first-principles calculations, we reveal that this giant optical anisotropy mainly comes from the linear (I3) structural units in a parallel arrangement, which maximizes the difference of polarizability along the different crystallographic axes. This work highlights the potential of natural polyiodide crystals as an outstanding platform to satisfy the increasing demand for photonic applications that exploit polarization in optical communication, three-dimensional imaging, ultrahigh-resolution sensing and other tasks.

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Fig. 1: Structure and optical images of C3H8N6I6·3H2O crystal.
The alternative text for this image may have been generated using AI.
Fig. 2: Visualized optical anisotropy of C3H8N6I6·3H2O.
The alternative text for this image may have been generated using AI.
Fig. 3: Dielectric and optical anisotropy of C3H8N6I6·3H2O.
The alternative text for this image may have been generated using AI.
Fig. 4: Comparison of birefringence.
The alternative text for this image may have been generated using AI.
Fig. 5: Theoretical analysis of C3H8N6I6·3H2O.
The alternative text for this image may have been generated using AI.

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Data availability

The authors declare that all data supplementary to the findings of this study are available within the paper and its Supplementary Information files. The X-ray crystallographic coordinates for structure reported in this study has been deposited at the Cambridge Crystallographic Data Centre (CCDC), under deposition number 2151897. These data can be obtained free of charge from The Cambridge Crystallographic Data Centre via www.ccdc.cam.ac.uk/data_request/cif. Any further relevant data are available from the authors upon reasonable request.

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Acknowledgements

We thank S. G. Zhao, J. H. Luo, and H. G. Gu for helpful discussions and experimental assistance. This work acknowledges the financial support from the National Natural Science Foundation of China (22122507 (S.Z.), 22193042 (J.L.) and 21921001 (J.L.)), Guangdong Basic and Applied Basic Research Foundation (grant no. 2023A1515030149) (H.G.), the Natural Science Foundation of Fujian Province (2022J02012) (S.Z.), the Youth Innovation Promotion Association of Chinese Academy of Sciences (Y202069) (S.Z.) and the Key Research Program of Frontier Sciences of the Chinese Academy of Sciences (ZDBS-LY SLH024) (J.L.).

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S.Z. and J.L. contributed to the conception of the research. M.H. provided suggestions for research. H.G. and S.L. guided and Z.G. performed the Mueller matrix spectroscopic ellipsometry analyses and CP analyses. Y.Z. performed the experiments and wrote the manuscript. Y.L., X.Z. and Y.S. assisted in the experimental and theoretical analysis. All authors discussed the results and reviewed the manuscript.

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Correspondence to Honggang Gu, Sangen Zhao or Junhua Luo.

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Nature Photonics thanks Kang Min Ok, Bingbing Zhang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–14 and Tables 1–7.

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The recorded images of crystals.

Supplementary Video 2 (download MP4 )

The recorded images of crystals.

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Zhou, Y., Guo, Z., Gu, H. et al. A solution-processable natural crystal with giant optical anisotropy for efficient manipulation of light polarization. Nat. Photon. 18, 922–927 (2024). https://doi.org/10.1038/s41566-024-01461-8

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