“…17 Under the guidance of these ideas, high-performance IR NLO materials with tetrahedron [MQ 4 ] n − as the NLO functional motif have been extensively studied, such as BaGa 4 Q 7 (Q = S, Se), 18,19 BaGa 2 MQ 6 (M = Si, Ge; Q = S, Se), 20 M II 3 P 2 S 8 (M II = Zn, Hg), 21,22 and AM II M IV Q 4 (A = Eu, Sr, Ba; M II = Mn, Zn, Cd, Hg; M IV = Si, Ge, Sn; Q = S, Se). 23–28 A common strategy for broadening band gaps is introducing alkali or alkaline earth metals to these compounds. However, the interaction between alkali or alkaline earth metal cations and anions ( i.e.…”