A pentanary chloride sulfate KBiCl 2 SO 4 (1) is synthesized via a simple solution routine. 1 is crystallized in the chiral orthorhombic P2 1 2 1 2 1 with Z = 4, and its onedimensional structure features a {[BiCl 2 (SO 4 )] − } ∞ chain along the polar axis. Its second-harmonic generation response is approximately 1.7 times that of KDP, and it can achieve phase matchability under the radiation of 1064 nm laser. Its optical energy gap is measured to be 3.95 eV. The density functional theory calculation results indicate that both [BiCl 2 O 3 □] 5− and [SO 4 ] 2− units serve as functional moieties for its promising nonlinear optical performance.

Chalcogenide borates were very rarely investigated in the past. As the second selenide borate, YSeBO 2 obtained by a high-temperature solid-state reaction crystallizes in the noncentrosymmetric orthorhombic space group Cmc2 1 with a novel structure type. Its structure consists of two basic building units, [BO 3 ] 3− planar triangles and [YO 3 Se 4 ] 11− pentagonal bipyramids, and features the [YSeBO 2 ] n planar belt. Second-harmonic-generation measurement shows its phase-matchable activity. YSeBO 2 has an optical energy gap of 3.45 eV. Density functional theory calculation is also performed, addressing the electronic structure and nonlinearoptical property.