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Herein, a novel optical crystal material, C8H6IN3O4, has been synthesized through rational design. Remarkably, C8H6IN3O4 showcases a large birefringence of 0.55@550 nm, surpassing those of commercially available birefringent materials. Theoretical calculations and analyses indicate that this phenomenon arises from the uniform alignment of π-conjugated [NO3] and [C8H6IN2O]+ groups.

Graphical abstract: C8H6IN3O4: a birefringent crystal induced by uniformly aligned hybrid groups

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