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Article Abstract
In recent years, planar π-conjugated systems have emerged as a pivotal platform for designing birefringent materials due to their intrinsic structural anisotropy. Among the documented π-conjugated motifs, pyridinium-derived cations exhibit exceptional anisotropic first-order polarizabilities, demonstrating remarkable potential for birefringence modulation. Herein, single crystals of (HCN)VO·2HO () were successfully synthesized via an aqueous solution method. In the crystal structure of , the unique (VO) group is constructed by five types of twisted (VO) octahedra connected by an edge-sharing mode. Besides, exhibits a moderate band gap of 2.33 eV, and its birefringence value reaches 0.219, which surpasses that of many vanadates (∼0.1). The first-principles calculations were further performed to elucidate its structure-property relationship.
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