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The structure of Zn<jats:sub>3<\/jats:sub>V<jats:sub>2<\/jats:sub>TeO<jats:sub>10<\/jats:sub> is a complicated three\u2010dimensional (3D) network constructed by the interconnection of ZnO<jats:sub>5<\/jats:sub>, ZnO<jats:sub>6<\/jats:sub>, VO<jats:sub>4<\/jats:sub>, and TeO<jats:sub>4<\/jats:sub> polyhedra via corner\u2010 and edge\u2010sharing. Cd<jats:sub>4<\/jats:sub>V<jats:sub>2<\/jats:sub>Te<jats:sub>3<\/jats:sub>O<jats:sub>15<\/jats:sub> with an acentric structure features a 3D network in which the cadmium tellurite layers are further interconnected by both \u201cisolated\u201d VO<jats:sub>4<\/jats:sub> tetrahedra and one\u2010dimensional (1D) vanadium oxide helical chains. Cd<jats:sub>4<\/jats:sub>V<jats:sub>2<\/jats:sub>Te<jats:sub>3<\/jats:sub>O<jats:sub>15<\/jats:sub> displays a second harmonic generation (SHG) efficiency of about 1.4 times that of KH<jats:sub>2<\/jats:sub>PO<jats:sub>4<\/jats:sub> (KDP). Both compounds are direct band\u2010gap semiconductors and are transparent in the range of 0.6\u201310.0\u2005\u03bcm. 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