Enhancement of birefringence is significant since the birefringent materials can create and control polarized light and be used extensively in various advanced optical systems. By optimizing the arrangement of [SbS] units with stereo-chemical active lone pair electrons, a new quaternary thioantimonate LiSrSbS with a large birefringence has been successfully synthesized by a high temperature solid-state reaction method. LiSrSbS crystallizes in the monoclinic space group of 2/. In the structure, the isolated infinite [LiS] chains and zigzag [SrS] chains are alternately connected with each other to compose a three-dimensional (3D) framework, and the isolated pyramid [SbS] units are located between them. To analyze the source of large birefringence, the electronic structure and optical properties of LiSrSbS were further investigated by the first-principles method, and the results show that the optimized arrangement [SbS] trigonal pyramid induces a large birefringence.
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