- In this work we present spectroscopic studies of a laser system which combines transition metal-doped crystal pumped by a dye-doped solid-state laser. A dye-doped solid state laser emitting at ∼610 nm was chosen to allow a better fit into the absorption peak of the LiCAF crystal, peaking at ∼625 nm, in order to increase the efficiency of the light absorption of the Cr+3 ions. The pump laser is a dye-doped solid state laser Red Perylimide Dye (RPD)-doped in a composite-glass. This lasing maximum is at ∼608 nm with a threshold energy of ∼0.3 mJ/pulse, and a lasing slope efficiency of ∼2.5% under excitation of 532 nm Nd:YAG laser. With the excitation of dye-doped solid state laser the Cr+3:LiCAF emission centered at ∼740 nm (due to the 4T2 → 4A2 transition) with lifetime of 170 μs and emission cross-section, σf, of 1.4 × 10−20 cm−2. The observed data allow us to plan a tunable Cr-crystal laser pumped by a solid-state dye laser.