The discovery of new nonlinear optical (NLO) materials for coherent light generation in the deep‐ultraviolet (DUV, wavelength below 200 nm) region is essential for the development of laser technologies. Herein, we report a new material CsB4O6F (CBF), which combines the superior structural properties of two well‐known NLO materials, β‐BaB2O4 (BBO) and KBe2BO3F2 (KBBF). CBF exhibits excellent DUV optical properties including a short cutoff edge (155 nm), a large SHG response (≈1.9×KDP), and a suitable birefringence that enables frequency doubling down to 171.6 nm. Remarkably, CBF melts congruently and shows an improved growth habit. In addition, our rational design strategy will contribute to the discovery of DUV NLO materials.

Two new cadmium sulfamates, namely, centrosymmetric Cd(NH2SO3)2·2H2O and noncentrosymmetric Cd(NH2SO3)2 have been successfully synthesized. Crystals of Cd(NH2SO3)2·2H2O grown by an aqua-solution method reveal an infinite chain structure consisting of trans-[CdO2(H2O)2(NH2)2]...