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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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.

Author information

Author notes

  1. These authors contributed equally: Shanyuan Niu, Graham Joe, Huan Zhao.

Affiliations

  1. Mork Family Department of Chemical Engineering and Materials Science, University of Southern California, Los Angeles, CA, USA

    • Shanyuan Niu
    • , Yucheng Zhou
    • , Thomas Orvis
    • , Huaixun Huyan
    • , Yang Liu
    • , Han Wang
    •  & Jayakanth Ravichandran
  2. Department of Electrical and Computer Engineering, University of Wisconsin–Madison, Madison, WI, USA

    • Graham Joe
    • , Jad Salman
    •  & Mikhail A. Kats
  3. Ming Hsieh Department of Electrical Engineering, University of Southern California, Los Angeles, CA, USA

    • Huan Zhao
    • , Jiangbin Wu
    • , Stephen B. Cronin
    • , Han Wang
    •  & Jayakanth Ravichandran
  4. Materials and Manufacturing Directorate, Air Force Research Laboratory, Wright-Patterson AFB, Dayton, OH, USA

    • Krishnamurthy Mahalingam
    • , Brittany Urwin
    •  & Brandon M. Howe
  5. J. A. Woollam Co. Inc., Lincoln, NE, USA

    • Thomas E. Tiwald
  6. Center for Electron Microscopy and Microanalysis, University of Southern California, Los Angeles, CA, USA

    • Matthew Mecklenburg
  7. Loker Hydrocarbon Research Institute and Department of Chemistry, University of Southern California, Los Angeles, CA, USA

    • Ralf Haiges
  8. Department of Physics and Astronomy, University of Missouri, Columbia, MO, USA

    • David J. Singh

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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.

Competing interests

The authors declare no competing interests.

Corresponding authors

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

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DOI

https://doi.org/10.1038/s41566-018-0189-1

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