“…Traditional NLO materials such as β-BaB 2 O 4 , LiB 3 O 5 , and LiNbO 3 are of limited usage in the mid-infrared regime due to strong multiphonon absorption. Currently, the commercially available infrared NLO crystals are AgGaS 2 , AgGaSe 2 ,and ZnGeP 2 . , They exhibit large NLO coefficients and a broad transmission range; however, they also suffer some intrinsic drawbacks such as a rather low laser induced damage threshold (LIDT) , and strong absorption of 1-2 μm, limiting the choice of pump lasers. , To qualify as a good NLO material, there are several criteria: (1) large SHG coefficients to have efficient NLO conversion; (2) wide transparency window allowing broad-band tunability; (3) large LIDT, and (4) phase-matchability for good SHG efficiency. ,− It is well known that the main challenge in the discovery and optimization of NLO materials is the tradeoff between the bandgap and the magnitude of the NLO coefficients: materials with larger bandgaps typically have lower SHG coefficients but higher LIDTs. , Finding new infrared NLO crystals with a superior optimized set of optical properties to the current materials is a grand challenge in this field.…”