With renewed refractive indices, the potential of a solid solution LiGaS 2 : LiGaSe 2 → LiGa(S 1−x Se x ) 2 ( x = 0 − 1) in optical frequency conversionespecially in phase matching and group velocity matching-is theoretically investigated, together with the composition ratio limitation. It is found that the solution has excellent features for generating coherent ultrafast mid-IR sources covering 8-11 μm, which can be realized by type II down-conversion in the ba-plane with perfect group velocity matching, or type I in the bc-plane with part group velocity matching. This will have broad applications in LiDAR monitoring and precision spectroscopy, as well as life and environmental sciences.