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Title: Colossal Optical Anisotropy from Atomic-Scale Modulations

Journal Article · · Advanced Materials
ORCiD logo [1];  [2];  [3];  [1];  [2];  [3];  [3];  [2];  [2];  [4];  [4];  [3];  [1];  [1];  [5];  [5];  [6]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of Wisconsin, Madison, WI (United States)
  2. Washington Univ., St. Louis, MO (United States)
  3. Univ. of Southern California, Los Angeles, CA (United States)
  4. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
  5. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  6. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
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Materials with large birefringence (Δn, where n is the refractive index) are sought after for polarization control (e.g., in wave plates, polarizing beam splitters, etc.), nonlinear optics, micromanipulation, and as a platform for unconventional light–matter coupling, such as hyperbolic phonon polaritons. Layered 2D materials can feature some of the largest optical anisotropy; however, their use in most optical systems is limited because their optical axis is out of the plane of the layers and the layers are weakly attached. This work demonstrates that a bulk crystal with subtle periodic modulations in its structure—Sr9/8TiS3—is transparent and positive-uniaxial, with extraordinary index ne = 4.5 and ordinary index no = 2.4 in the mid- to far-infrared. The excess Sr, compared to stoichiometric SrTiS3, results in the formation of TiS6 trigonal-prismatic units that break the chains of face-sharing TiS6 octahedra in SrTiS3 into periodic blocks of five TiS6 octahedral units. The additional electrons introduced by the excess Sr form highly oriented electron clouds, which selectively boost the extraordinary index ne and result in record birefringence (Δn > 2.1 with low loss). The connection between subtle structural modulations and large changes in refractive index suggests new categories of anisotropic materials and also tunable optical materials with large refractive-index modulation.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); US Department of the Navy, Office of Naval Research (ONR); US Army Research Office (ARO); National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
2439947
Journal Information:
Advanced Materials, Journal Name: Advanced Materials Journal Issue: 42 Vol. 35; ISSN 0935-9648
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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36 MATERIALS SCIENCE
birefringence
chalcogenides
optical anisotropy
structural modulation