“…Among them, π-conjugated groups may be the most important and successful, owing to their large optical anisotropy and remarkable microscopic second-order susceptibility, which promotes the discovery of some commercialized crystals, such as KBe 2 BO 3 F 2 (KBBF) with a (BO 3 ) 3– group, β-BaB 2 O 4 (BBO) with a (B 3 O 6 ) 3– group, and LiB 3 O 5 with a (BO 3 ) 3– group. − Especially since 2017, our group first studied the microscopic properties of large π-conjugated cyanurate (C 3 N 3 O 3 ) 3– , thus greatly triggering the rapid developments in this field . A succession of new crystals, including K 6 Cd 3 (C 3 N 3 O 3 ) 4 , KLi(HC 3 N 3 O 3 )·2H 2 O, , Cs 3 Na(H 2 C 3 N 3 O 3 ) 4 ·3H 2 O, and LiCl·(H 3 C 3 N 3 O 3 ), were discovered and grown. In addition, some new π-conjugated groups were immediately explored by many research groups, − e.g., (C 3 H 7 N 6 ) + , (C 5 H 6 ON) + , (C 4 H 6 N 3 ) + , [C(NH 2 ) 3 ] + , (HC 4 O 4 ) − , (C 6 N 9 ) 3– , (HC 3 N 3 S 3 ) 2– , and (H 2 C 4 N 2 O 3 ) 2– .…”