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Giant optical anisotropy in a quasi-one-dimensional crystal

An Author Correction to this article was published on 08 September 2021

This article has been updated

Abstract

Optical anisotropy is a fundamental building block for linear and nonlinear optical components such as polarizers, wave plates, and phase-matching elements1,2,3,4. In solid homogeneous materials, the strongest optical anisotropy is found in crystals such as calcite and rutile5,6. Attempts to enhance anisotropic light–matter interaction often rely on artificial anisotropic micro/nanostructures (form birefringence)7,8,9,10,11. Here, we demonstrate rationally designed, giant optical anisotropy in single crystals of barium titanium sulfide (BaTiS3). This material shows an unprecedented, broadband birefringence of up to 0.76 in the mid- to long-wave infrared, as well as a large dichroism window with absorption edges at 1.6 μm and 4.5 μm for light with polarization along two crystallographic axes on an easily accessible cleavage plane. The unusually large anisotropy is a result of the quasi-one-dimensional structure, combined with rational selection of the constituent ions to maximize the polarizability difference along different axes.

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Fig. 1: Structure and chemistry of BaTiS3.
Fig. 2: Structural, vibrational and chemical characterization of BaTiS3.
Fig. 3: Optical anisotropy.

Change history

  • 08 September 2021

    A Correction to this paper has been published: https://doi.org/10.1038/s41566-021-00875-y

  • 25 February 2022

    In the version of this article corrected 8 September 2021, there was an extraneous key in Fig. 3b, and the y-axis values and baseline in Fig. 3d were reoriented from “0.5 to −1.0” to “1.0 to −0.5”.

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Acknowledgements

The authors thank A. R. Tanguay and A. Madhukar for discussions, and technical assistance by T. Aoki and N. Bozdin. J.R. acknowledges USC Viterbi School of Engineering Startup Funds and support from the Air Force Office of Scientific Research under award no. FA9550-16-1-0335. S.N. acknowledges Link Foundation Energy Fellowship. M.A.K. acknowledges support from the Office of Naval Research (grant no. N00014-16-1-2556). H.W. acknowledges support from the Army Research Office (grant no. W911NF-16-1-0435) and National Science Foundation (grant no. ECCS-1653870). Work at the University of Missouri (D.J.S.) was supported by the Department of Energy, Basic Energy Sciences through the Solid-State Solar Thermal Energy Conversion Center, an Energy Frontier Research Center, under award no. DE-SC0001299/DE-FG02-09ER46577. S.B.C. acknowledges support from the Department of Energy under award no. DE-FG02–07ER46376. The studies at Air Force Research Laboratory were supported by the Air Force Office of Scientific Research under award no. FA9550-15RXCOR198. The authors acknowledge the use of facilities at the Center for Electron Microscopy and Microanalysis at the University of Southern California and the Irvine Materials Research Institute at the University of California, Irvine.

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Contributions

J.R. conceived and supervised the research with M.A.K. M.A.K. identified the large optical anisotropy. H.W. supervised the Raman and infrared spectroscopy studies. S.N., Y.Z. and H.H. built the apparatus and grew the crystals. S.N., Y.L. and T.O. performed structural and chemical characterizations. R.H. contributed single-crystal X-ray diffraction measurements. M.M., K.M., B.U. and B.M.H. contributed TEM studies. S.N., H.Z. and J.W. studied the Raman response. G.J., H.Z. and J.S. performed infrared spectroscopy. G.J. and T.E.T. performed ellipsometry studies. D.J.S. contributed theoretical calculations. All authors discussed the results. S.N., M.A.K. and J.R. wrote the manuscript with contributions from all authors.

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Correspondence to Han Wang, Mikhail A. Kats or Jayakanth Ravichandran.

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Niu, S., Joe, G., Zhao, H. et al. Giant optical anisotropy in a quasi-one-dimensional crystal. Nat. Photon. 12, 392–396 (2018). https://doi.org/10.1038/s41566-018-0189-1

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