Two noncentrosymmetric metal chalcogenides,BaCdSnS4 and Ba3CdSn2S8,were synthesized using a high-temperature solid-state reaction in evacuated silica tube.Although two compounds have the same building units in their structures,namely CdS4,SnS4 and BaS8 units,both of them have different structures.BaCdSnS4 crystallizes in the orthorhombic space group Fdd2 and its structure can be characterized by the two-dimensional ∞[Cd-Sn-S] layers composed of corner-and edge-sharing CdS4 and SnS4 tetrahedra with Ba atoms located between the two adjacent ∞[Cd-Sn-S] layers.Ba3CdSn2S8 crystallizes in the space group I 4 3d of the orthorhombic system and the CdS4 and SnS4 groups are connected with each other via corner-sharing to form a three-dimensional framework,which is different from the 2D ∞[Cd-Sn-S] layer structure in BaCdSnS4.The UV-Vis-NIR diffuse-reflectance spectra show that the experimental band gaps are about 2.30 eV for BaCdSnS4 and 2.75 eV for Ba3CdSn2S8,respectively.IR and Raman measurement results indicate that their transparent ranges are up to 25 μm.Second-order NLO measurements show that BaCdSnS4 exhibits a strong powder second-harmonic generation(SHG)intensities at 2.09 μm laser pumping that are~5 and 0.7 times that of AgGaS2 in the particle size 38-55 and 150-200 μm,respectively,whereas Ba3CdSn2S8 only exhibits SHG intensities of about 0.8 and 0.1 times that of AgGaS2 at the same particle sizes.The origin of NLO response in BaCdSnS4 may originates from the macroscopic arrangement of the SnS4 and CdS4 tetrahedra.Furthermore,the photoluminescent properties of two compounds have also been investigated and show obvious blue and green light emission.