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Stereochemically active lone-pair (SCALP) cations are attractive units forrealizing optical anisotropy. Antimony (III) chloride perovskites with SCALPhave remained largely unknown till date. We synthesized vacancy orderedCs3Sb2Cl9 perovskite single crystals with SbCl6 octahedral linkage containingSCALP. Remarkably, Cs3Sb2Cl9 single crystals exhibit an exceptionalbirefringence of 0.12 +(-) 0.01 at 550 nm, which is the largest among pristineall-inorganic halide perovskites. The SCALP brings a large local structuraldistortion of the SbCl6 octahedra promoting birefringence optical responses inCs3Sb2Cl9 single crystals. Theoretical calculations reveal that theconsiderable hybridization of Sb 5s with Sb 5p and Cl 3p states largelycontribute to the SCALP. Furthermore, the change in the Sb-Cl-Sb bond anglecreates distortion in the SbCl6 octahedral arrangement in the apical andequatorial directions within the crystal structure incorporating the requiredanisotropy for the birefringence. This work explores pristine inorganic halideperovskite single crystals as a potential birefringent material with prospectsin integrated optical devices.

Stereochemically Active Lone-pair Leads to Strong Birefringence in the Vacancy Ordered Cs3Sb2Cl9 Perovskite Single Crystals