ABSTRACT Short‐wave ultraviolet (200–280 nm) nonlinear optical (NLO) crystals are scarce. Herein, by mixing two types of hetero‐coordinate substituted groups, we synthesized two new crystals, Zn(C 2 H 4 NO 2 ) 2 (SO 2 CH 3 NH 2 ) 2 (ZGlyM) and Zn(C 2 H 4 NO 2 ) 2 SO 2 (NH 2 ) 2 (ZGlyS), featuring a unique ZnO(C 2 H 4 NO 2 ) 2 secondary functional building unit which tends to assemble into a polar chain. Interestingly, disorder in ZGlyM results in a centrosymmetric structure, whereas in ZGlyS, the replacement of the polar tetrahedral group eliminates disorder and preserves a non‐centrosymmetric structure. Notably, the ZGlyS exhibits a rare balance between a short UV cutoff edge of 209 nm, a large second harmonic generation effect of 1.36 × KH 2 PO 4 , and a large birefringence of 0.126@546 nm. Remarkably, its phase‐matching range covers the entire transparent wavelength range, namely, the shortest phase‐matching wavelength is 209 nm. This work provides a potential short‐wave UV NLO crystal and offers new insights for the design of such crystals.
Chenjie et al. (Fri,) studied this question.