Abstract
Large birefringence is a crucial but hard-to-achieve optical parameter that is a necessity for birefringent crystals in practical applications involving modulation of the polarization of light in modern opto-electronic areas. Herein, an oxyanion polymerization strategy that involves the combination of two different types of second-order Jahn-Teller distorted units is employed to realize giant anisotropy in a covalent molybdenum tellurite. Mo(H2O)Te2O7 (MTO) exhibits a record birefringence value for an inorganic UV-transparent oxide crystalline material of 0.528 @ 546nm, which is also significantly larger than those of all commercial birefringent crystals. MTO has a UV absorption edge of 366nm and displays a strong powder second-harmonic generation response of 5.4 times that of KH2PO4. The dominant roles of the condensed polytellurite oxyanions [Te8O20]8- in combination with the [MoO6]6- polyhedra in achieving the giant birefringence in MTO are clarified by structural analysis and first-principles calculations. The results suggest that polymerization of polarizability-anisotropic oxyanions may unlock the promise of birefringent crystals with exceptional birefringence.
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