Publication date: 28th August 2024
Stereochemically active lone pair (SCALP) cations are attractive units for realizing optical anisotropy. Antimony(III) chloride perovskites with the SCALP have remained largely unknown to date. We synthesized a new vacancy ordered Cs3Sb2Cl9 perovskite single crystals with SbCl6 octahedral linkage containing the SCALP. Remarkably, all-inorganic halide perovskite Cs3Sb2Cl9 single crystals exhibit an exceptional birefringence of 0.12 ± 0.01 at 550 nm. The SCALP brings a large local structural distortion of the SbCl6 octahedra promoting birefringence optical responses in Cs3Sb2Cl9 single crystals. Theoretical calculations reveal that the considerable hybridization of Sb 5s and 5p with Cl 3p states largely contributes to the SCALP. Furthermore, the change in the Sb−Cl−Sb bond angle creates distortion in the SbCl6 octahedral arrangement in the apical and equatorial directions within the crystal structure incorporating the required anisotropy for the birefringence. This work explores pristine inorganic halide perovskite single crystals as a potential birefringent material with prospects in integrated optical devices.
We acknowledge Science and Engineering Research Board (SERB) grant SERB-STAR grant STR/2020/000053 for financial support. AM thanks to the Council of Scientific and Industrial Research (CSIR, Project No: 01(3031)/21/EMR-II) and SK thanks CSIR for the research fellowship. SA and ID acknowledge Technical Research Centre (TRC), IACS for instrumental and computational support.
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