Colossal Optical Anisotropy from Atomic-Scale Modulations

Hongyan Mei, Guodong Ren, Boyang Zhao, Jad Salman, Gwan Yeong Jung, Huandong Chen, Shantanu Singh, Arashdeep S. Thind, John Cavin, Jordan A. Hachtel, Miaofang Chi, Shanyuan Niu, Graham Joe, Chenghao Wan, Nick Settineri, Simon J. Teat, Bryan C. Chakoumakos, Jayakanth Ravichandran, Rohan Mishra, Mikhail A. Kats

Research output: Contribution to journalArticlepeer-review

13 Scopus citations

Abstract

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.

Original languageEnglish
Article number2303588
JournalAdvanced Materials
Volume35
Issue number42
DOIs
StatePublished - Oct 19 2023

Funding

The work at UW‐Madison was supported by ONR, with award no. N00014‐20‐1‐2297. The work at USC and WUStL were supported, in part, by an ARO MURI program with award no. W911NF‐21‐1‐0327, and the National Science Foundation (NSF) of the United States under grant numbers DMR‐2122070 and DMR‐2122071. J.R. acknowledges support from the Army Research Office under Award No. W911NF‐19‐1‐0137, and an Air Force Office of Scientific Research grant no. FA9550‐22‐1‐0117. This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under contract no. DE‐AC02‐05CH11231. J.R., B.Z., and H.C. gratefully acknowledge the use of Core Center for Excellence in Nano Imaging (CNI), University of Southern California for some of the sample preparation and characterization studies. R.M. acknowledges NSF for partial support through grant DMR‐2145797. M.K. and H.M. acknowledge the use of facilities and instrumentation at the UW‐Madison Wisconsin Centers for Nanoscale Technology (WCNT) partially supported by the NSF through the University of Wisconsin Materials Research Science and Engineering Center (DMR‐1720415). STEM characterization was performed at the Center for Nanophase Materials Sciences and X‐ray structural work at the Spallation Neutron Source, both of which are US Department of Energy, Office of Science User Facility operated by Oak Ridge National Laboratory. This work used computational resources through allocation DMR160007 from the Advanced Cyberinfrastructure Coordination Ecosystem: Services & Support (ACCESS) program, which is supported by NSF grants #2138259, #2138286, #2138307, #2137603, and #2138296. The work at UW-Madison was supported by ONR, with award no. N00014-20-1-2297. The work at USC and WUStL were supported, in part, by an ARO MURI program with award no. W911NF-21-1-0327, and the National Science Foundation (NSF) of the United States under grant numbers DMR-2122070 and DMR-2122071. J.R. acknowledges support from the Army Research Office under Award No. W911NF-19-1-0137, and an Air Force Office of Scientific Research grant no. FA9550-22-1-0117. This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under contract no. DE-AC02-05CH11231. J.R., B.Z., and H.C. gratefully acknowledge the use of Core Center for Excellence in Nano Imaging (CNI), University of Southern California for some of the sample preparation and characterization studies. R.M. acknowledges NSF for partial support through grant DMR-2145797. M.K. and H.M. acknowledge the use of facilities and instrumentation at the UW-Madison Wisconsin Centers for Nanoscale Technology (WCNT) partially supported by the NSF through the University of Wisconsin Materials Research Science and Engineering Center (DMR-1720415). STEM characterization was performed at the Center for Nanophase Materials Sciences and X-ray structural work at the Spallation Neutron Source, both of which are US Department of Energy, Office of Science User Facility operated by Oak Ridge National Laboratory. This work used computational resources through allocation DMR160007 from the Advanced Cyberinfrastructure Coordination Ecosystem: Services & Support (ACCESS) program, which is supported by NSF grants #2138259, #2138286, #2138307, #2137603, and #2138296.

Keywords

  • birefringence
  • chalcogenides
  • optical anisotropy
  • structural modulation

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