“…The investigation of new second-order nonlinear optical (NLO) materials has attracted considerable attention due to the important applications of these materials in optoelectronic technologies, such as in optical parametric oscillators (OPO), difference frequency generation (DFG), laser frequency conversion, and signal communication. 1,2 Significant efforts have been made to develop new NLO crystals, and in the past few years many new inorganic NLO crystals have been synthesized, including some metal chalcogenides (e.g., APSe 6 (A = K, Rb), 3,4 AAsQ 2 (A = Li, Na; Q = S, Se), 5,6 AZrPQ 6 7,8 and A 4 GeP 4 Q 12 (A = K, Rb, Cs; Q = S, Se), 9 Ln 4 GaSbS 9 (Ln = Pr, Nd, Sm, Gd-Ho), 10 and Ln 3 GaS 6 (Ln = Dy, Y) 11 ), halides (e.g., Rb 2 CdBr 2 I 2 , 12 Cs 2 HgI 2 Cl 2 , 13 Hg 2 Br 3 I, 14 and HgBrCl 15 ), and borates (e.g., NaSr 3 Be 3 B 3 O 9 F 4 , 16 Na 2 Be 4 B 4 O 11 and LiNa 5 Be 12 B 12 O 33 , 17 Ba 4 B 11 O 20 F, 18 Cd 5 B 3 O 9 F, 19 and K 3 B 6 O 10 Br 20 ). A NLO crystal with excellent performance requires several conditions to be satisfied, including a high coefficient of second-order harmonic generation (SHG), a wide transparent region, good phase matchability, a moderate laser damage threshold, and the availability of the corresponding large-size crystal.…”