“…[1][2][3][4][5][6] Based on their operating regions, NLO materials can be classified into deep-ultraviolet (DUV), ultraviolet-visible to near-infrared (UV-vis-NIR), and mid-to far-infrared (IR) NLO materials. In the past few decades, a large number of excellent oxide-based UV or DUV NLO materials, including β-BaB 2 O 4 , 7 LiB 3 O 5 , 8 KH 2 PO 4 , 9 KTiOPO 4 , 10,11 KBe 2 BO 3 F 2 12 and NH 4 B 4 O 6 F, 13 have been rationally designed and fabricated, [14][15][16][17] while for mid-and far-IR bands, the commercialized NLO materials are composed of chalcopyrite-like AgGaS 2 (AGS), AgGaSe 2 (AGSe) and ZnGeP 2 (ZGP). [18][19][20] Nevertheless, due to the intrinsic drawbacks of these materials, such as the low laser-induced damage threshold (LIDT) in AGS and AGSe, 21 the non-phase matching behavior of AGSe and strong twophoton absorption in ZGP at around ∼1 μm, their applications are highly limited.…”