“…Inorganic nonlinear optical (NLO) materials play a crucial role in expanding the spectral range of solid-state laser through frequency conversion technology, owing to their excellent NLO properties, such as large nonlinear coefficients, wide transparent windows, good thermal and chemical stabilities, and so forth. − Among them, metal selenites and tellurites are more likely to form non-centrosymmetric (NCS) structure as the prerequisite of second-harmonic generation (SHG) property, due to the stereochemically active lone pairs on Se 4+ or Te 4+ cation susceptible to second-order Jahn–Teller (SOJT). During the past two decades, through the combination of distorted octahedrally coordinated d 0 transition metal with Se 4+ and Te 4+ cations, a large number of compounds with excellent SHG properties have been discovered, such as β-BaTeMo 2 O 9 (600 × α-SiO 2 ), Na 2 TeW 2 O 9 (500 × α-SiO 2 ), , Cs 2 TeW 3 O 12 (400 × α-SiO 2 ), − and A 2 (MoO 3 ) 3 (SeO 3 ) (A = Tl, NH 4 ) (400 × α-SiO 2 ) . Nonetheless, the majorities of them are of small band gaps ( E g ) and complex chemical compositions, which hinder their applications in UV–visible region; also, their bulk single-crystal growths are difficult.…”